Research Article Vol. 30, No.

4 / 14 Feb 2022 / Optics Express 5222

Advances in mid-infrared spectroscopy enabled

by supercontinuum laser sources
I VAN Z ORIN , * PAUL G ATTINGER , A LEXANDER E BNER , AND
M ARKUS B RANDSTETTER
Research Center for Non-Destructive Testing, Science Park 2, Altenberger Str.69, 4040 Linz, Austria
* ivan.zorin@recendt.at

Abstract: Supercontinuum sources are all-fiber pulsed laser-driven systems that provide high
power spectral densities within ultra-broadband spectral ranges. The tailored process of generating
broadband, bright, and spectrally flat supercontinua—through a complex interplay of linear and
non-linear processes—has been recently pushed further towards longer wavelengths and has
evolved enough to enter the field of mid-infrared (mid-IR) spectroscopy. In this work, we review
the current state and perspectives of this technology that offers laser-like emission properties and
instantaneous broadband spectral coverage comparable to thermal emitters. We aim to go beyond
a literature review. Thus, we first discuss the basic principles of supercontinuum sources and then
provide an experimental part focusing on the quantification and analysis of intrinsic emission
properties such as typical power spectral densities, brightness levels, spectral stability, and beam
quality (to the best of the authors’ knowledge, the M2 factor for a mid-IR supercontinuum source
is characterized for the first time). On this basis, we identify key competitive advantages of
these alternative emitters for mid-IR spectroscopy over state-of-the-art technologies such as
thermal sources or quantum cascade lasers. The specific features of supercontinuum radiation
open up prospects of improving well-established techniques in mid-IR spectroscopy and trigger
developments of novel analytical methods and instrumentation. The review concludes with a
structured summary of recent advances and applications in various routine mid-IR spectroscopy
scenarios that have benefited from the use of supercontinuum sources.

© 2022 Optica Publishing Group under the terms of the Optica Open Access Publishing Agreement

1. Introduction
Mid-infrared (mid-IR) spectroscopy is a lab-standard non-destructive analytical technique that
enables qualitative and quantitative chemical analysis of samples in all states of aggregation.
The keystone of mid-IR spectroscopic methods is the study of the interaction of polychromatic
mid-IR radiation with the matter under examination. The mid-IR spectral band spans the range
from 4000 cm−1 to 400 cm−1 (2.5 µm- 25 µm). Interpretation and analysis of measured spectra
provide insight into the structure of molecules (e.g., atomic masses and bond strengths) and
enable quantification of concentration [1]. Hence, mid-IR light sources are the workhorses that
form the technological ground for mid-IR spectroscopic measurements. This work reviews the
novel technology of mid-IR supercontinuum laser sources as an alternative to state-of-the-art
light emitters in this specific field.
In most routine scenarios, mid-IR spectrometers exploit thermal emitters (silicon carbide
elements—Globars) that are well-developed, robust, stable, and cost-effective. These classical
sources have reached their emission capabilities during the rapid evolution of the instrumental
basis in the last century, which was primarily aimed at detectors [2] and advancements of methods
(e.g. establishment of Fourier-domain IR spectroscopy, FTIR [3]). Further improvement of
thermal sources is challenging as it requires a significant temperature increase. However, it is
possible, as demonstrated by the technology of non-classical laser-driven plasma sources [4].
Thermal sources emit quasi-black-body radiation with a power spectral density (PSD) described
by Planck’s law. Their spectral coverage is well suited for most mid-IR spectroscopic applications.

#447269 https://doi.org/10.1364/OE.447269
Journal © 2022 Received 29 Oct 2021; revised 15 Dec 2021; accepted 15 Dec 2021; published 3 Feb 2022
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5223

However, they impose several fundamental limitations. Thermal emitters are spatially incoherent,
omni-directional and provide relatively low output optical power levels. This cumulatively leads
to deficient brightness (the term owes its usage to laser physics [5], also known as spectral
radiance). The practical importance of brightness should not be neglected in optical metrology,
and particularly in spectroscopic measurements. The brightness of a light source directly affects
the spectral power incident on the sample unit surface area. For mid-IR spectroscopy it means that,
according to the Beer’s law, the light-matter interaction path lengths can be extended preventing
total light attenuation and more molecules can be investigated. Thus, limits of detection can be
lowered. On the other hand, in photothermal applications, the signal is directly proportional to
the intensity of the incident light. Here, sufficient brightness is even more beneficial.
The invention and development of the laser provided an advanced high-brightness source
devoid of the disadvantages of thermal emitters [5,6]. Lasers possess high spatial coherence
(the emission mode area is small and formed by spatially correlated field patterns in contrast
to extended thermal sources), directionality, high output optical powers and beam qualities.
As a result, the brightness of laser sources is several orders of magnitude higher than that of
thermal emitters [5,7]. Since lasers are quasi-monochromatic, they had to be widely adapted
for mid-IR spectroscopic applications. The first systems were developed to provide tunable
emission (tailoring the emission wavelength by modifying system parameters or environmental
conditions). Thereby, tunable small band-gap lead-salt diode lasers covering the entire mid-IR
spectral range [8,9] have been applied for spectroscopic measurements already in the mid-60s.
These systems have verified the expectations on high-brightness sources in mid-IR spectroscopy
[10–12]. However, they were not widespread due to the relatively low power levels (typically
several hundred microwatts), inferior beam properties (high divergence, astigmatic emission), and
strict operation requirements (cryogenic cooling is necessary to achieve population inversion) [13].
Diode lasers based on lead-salt heterostructures were soon followed by antimonide diode lasers
[14–17], laser sources based on parametric frequency conversion (optical parametric oscillators,
difference frequency generators) [18,19], and adapted solid-state lasers [20]. These laser systems
have resolved the limitations of the first designs. They offered—depending on the class of the
emitters—particular advantages such as high output powers, room-temperature operation, and
relative simplicity of the design. Conversion systems and solid-state lasers were capable of
fundamental mode emission. In terms of spectral coverage, the range from 2.3 µm to about 5
µm became available for lasers at this time. Nevertheless, probably the major milestone towards
advanced laser-based mid-IR spectroscopy has been made with the development of the band
engineered semiconductor laser (based on intersubband transitions), namely the quantum cascade
laser (QCL) [21]. In contrast to the above-mentioned systems, high brightness mid-IR QCLs
have demonstrated particular application advantages due to their robustness, stable operation at
room temperatures, compact dimensions and wide spectral tunability (several chips can be united
in one emitter to expand the spectral coverage further). QCLs feature a narrow spectral linewidth
and relatively high output average powers. The QCL technology virtually covers the entire
mid-IR range. Through these particular strengths, QCL systems have gained widespread use,
facilitating highly sensitive mid-IR spectroscopic measurements since fundamental and strong
absorption bands can be probed, which were poorly accessible at the time for other laser systems.
As a result, QCLs have become a standard tool in laser-based mid-IR absorption spectroscopy.
They led to development and improvement of methods in various molecular fingerprinting fields
such as process monitoring, gas tracing, and biomedical spectroscopy, laboratory scenarios
etc.—as evidenced by recent extensive scientific reviews [22–24]. Nowadays, progress in mid-IR
laser spectroscopy has not stopped and continues to impress. For example, in addition to
increased sensitivity through high brightness sources, spectral resolution and accuracy can also be
significantly enhanced by using frequency-comb lasers in dual-comb spectroscopy [25]. Beyond
lasers, infrared synchrotron sources are worth mentioning, as they offer high-brightness levels in
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5224

ultra-broad spectral ranges [26]. These sources are superior to conventional thermal emitters in
various mid-IR spectroscopic applications [27–29]. However, the practical use of synchrotrons is
limited and they are unlikely to become standard laboratory equipment due to inflexibility and
extreme operating costs. In the following sections, we exhibit the capabilities of supercontinuum
sources that have laser properties and high brightness beyond that of synchrotrons, for this reason
supercontinuum lasers are called table-top synchrotrons in [30]. Our analysis and comparisons
(e.g. of brightness levels) focus on the most established and gold-standard representatives: the
state-of-the-art QCLs and conventional thermal sources.
The phenomenon of supercontinuum generation—the process underlying supercontinuum
sources—was first observed and reported in 1970 [31] (the term has been introduced in [32])
in an experiment, which has been enabled by high peak power lasers. A continuous optical
spectrum spanning the entire visible range has been produced via spectral broadening during
the propagation of intense picosecond laser pulses (Q-switched mode-locked Nd:Glass laser,
530 nm wavelength, frequency-doubled in a potassium dihydrogen phosphate crystal) through
bulk borosilicate glass. Hereinafter, driven primarily by interests of spectroscopy, supercontinua
have been generated in various bulk dielectric media [33–35]. The processes behind spectral
broadening were intensively studied, interpreted and tailored. The most significant milestone in
the commercialization and establishment of supercontinuum sources as versatile and flexible
metrological tools was passed with the transition to another generation platform, namely optical
fibers [36–40]. During the last decades, supercontinuum sources have been rapidly evolving.
Currently, the focus is still on taking control of the generation process and stabilization of their
emission [41] (potentially switching to all-normal dispersion pumping regime [42–53]). At the
same time, numerous efforts are made to increase optical output power levels (especially in the
mid-IR spectral range [54–58]), and to extend the spectral coverage primarily to the mid-IR
[59–68], but also to the ultraviolet [49,69–71] range. An impressive example of the progress
in this field is the recent rapid evolution of fluoride ZBLAN [ZrF4 -BaF2 -LaF3 -AlF3 -NaF] fiber
based supercontinuum generators. Initially starting with a few milliwatts of output optical power
[72,73] these sources have recently reached levels of tens of watts [74]. A closer look at the
mid-IR spectral window reveals that various aspects of the multifaceted topic of supercontinuum
generation are being studied by groups from different fields. Significant efforts are currently being
made to expand the operational spectral window. For instance, the implementation of cascaded
schemes emerged as a promising solution to achieve high spectral performance, particularly in
terms of bandwidth and brightness [75–80]. Besides, studies of supercontinuum generation
processes and their controlled tailoring [37,39,42,44,46,76,81–102] are still fundamental research
topics. In order to generate and handle the long-wavelength supercontinua, glass materials are
being optimized. Material research has mainly focused on glasses with wide mid-IR transparency:
tellurite [103], fluoride [56,57,74,104–107]), and chalcogenide glasses [60,68,75,108–122].
Moreover, already developed system architectures are being optimized and technically adapted
[123]. As a result, several reports of ultra-broadband and bright supercontinuum generation
in the mid-IR have recently been presented [60,66,68,124]. In contrast, this work reviews
the current maturity state of the mid-IR fiber-based supercontinuum technology beyond these
generation-related subjects—in the applied field of mid-IR spectroscopy—and discusses core
concepts, principles, particular emission properties as well as prospects and potential application
scenarios.

2. Mid-IR supercontinuum technology

The modern mid-IR supercontinuum laser source is a prominent representative of fiber-based
emitters [125]. Mid-IR supercontinua provide instantaneous ultra-broadband spectral coverage
(more than an octave). The supercontinuum generation process is rooted in the complex meshing
and co-action of linear and nonlinear processes occurring during the propagation of intense
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5225

pulses in the optical fiber. Depending on the pump scheme, material parameters, fiber geometry,
dispersion regime, and input pulse duration, the ensemble of phenomena and mechanisms
responsible for spectral broadening can significantly vary, certain processes can dominate or
be suppressed by others. The major nonlinear contributors to the process of supercontinuum
generation are [126]: stimulated Raman scattering, self-phase modulation, four-wave mixing,
modulation instability, cross-phase modulation, soliton dynamics (soliton fission and soliton
self-frequency shift) and dispersive wave generation (extensive overviews on this topic can be
found e.g. in [36,38,39,127]).
Despite the sophisticated fundamental physics behind supercontinuum generation, the practical
realization for the mid-IR supercontinuum generation is relatively simple. Figure 1 illustrates
this point and depicts the conceptual principles and system architecture of a commercial fluoride
fiber based (InF3 ) supercontinuum generator. The system presented in Fig. 1 was developed,
reported and described in [106]. The pump system of the supercontinuum source is based on a
high peak power femtosecond mode-locked fiber laser. The laser radiates in the spectral range of
the opto-communication wavelengths of 1550 nm, where optical technology is well-developed.
The emitted laser pulses (50 MHz repetition rate) are amplified by an Er-doped fiber amplifier
and launched into a nonlinear fiber that transfers the pulse energy to the 1.9 µm spectral range,
corresponding to theand
dispersion regime, zero-dispersion wavelength
input pulse duration, of the designed
the ensemble fluorideand
of phenomena fiber. The second
mechanisms
amplification
responsible for stage implies
spectral a boost can
broadening of the optical power
significantly in the processes
vary, certain spectral range of around
can dominate or 2
µm (to >0.5 W average power levels) using the following forward-direction Thulium-doped
be suppressed by others. The major nonlinear contributors to the process of supercontinuum
generation are [126]:
cladding-pumped fiberstimulated Raman
amplifier (793 nmscattering, self-phase
pump diode). modulation,the
To compensate four-wave
anomalousmixing,
group
modulation instability, cross-phase modulation, soliton dynamics (soliton fission and soliton
velocity dispersion of the Tm-doped and the delivery fibers, a dispersion compensating fiber is
self-frequency shift) and dispersive wave generation (extensive overviews on this topic can be
pre-employed finalizing the pump system dealing with the time-frequency adaptation of optical
found e.g. in [36, 38, 39, 127]).
pulses for supercontinuum generation. Thereby, the shifted and spectrally pre-broadened pulses
Despite the sophisticated fundamental physics behind supercontinuum generation, the practical
consisting of for
realization trains
the of solitons
mid-IR are being coupled
supercontinuum into theis50
generation cm longsimple.
relatively InF3 fiber, where
Figure substantial
1 illustrates
broadening occurs. The generated supercontinuum radiation spanning the spectral
this point and depicts the conceptual principles and system architecture of a commercial fluoriderange from
1.25 µm to 4.6 µm is finally collimated by the output off-axis parabolic mirror.
fiber based (InF3 ) supercontinuum generator. The system presented in Fig. 1 was developed,

Source diagram
Emission spectrum Er-doped Tm-doped
Pump laser (fs) amplifier amplifier InF3 fiber
Isolator
PSD (dBm/nm)

1550 nm

Nonlinear Dispersion Coupling Output

fiber compensating to fluoride (collimator)
fiber fiber
Collimator
PSD
Spectral evolution within InF3 fiber (dBm/nm)
Wavelength (µm) 200
Propagation distance (cm)

5
0
r 150
fibe -5
-10
Supercontinuum source F3
In 100 -15
Grating pump system
-20
for illustrative -25
purposes
r 50
ea -30
nlin -35
No 0 -40
1 1.5 2 2.5 3 3.5 4 4.5
Wavelength (µm)

1. 1.Basic
Fig.Fig. Basicscheme
scheme and operatingprinciples
and operating principlesofof a mid-IR
a mid-IR supercontinuum
supercontinuum sourcesource
exemplified for afor
exemplified InF fiber
a 3InF based system: the depicted emission spectrum corresponds to the
3 fiber based system: the depicted emission spectrum corresponds
commercial supercontinuum
to the commercial generator
supercontinuum (Thorlabs,
generator SC4500,
(Thorlabs, fiber length
SC4500, of 50ofcm,
fiber length 50 MHz
50 cm,
repetition
50 MHz rate, 300 mW
repetition average
rate, 300 mWoutput power);
average outputthe simulated
power); spectral spectral
the simulated evolution of the pump
evolution
pulseofover the 200
the pump pulsecmoverlength InFcm
the 200 3 fiber—serves to illustrate to
length InF3 fiber—serves the mechanism
illustrate of generation;
the mechanism
the source architecture
of generation; and spectral
the source evolution
architecture are adapted
and spectral from are
evolution [106] with permission
adapted from [106] from
OSA.with permission from OSA.

reported and described in [106]. The pump system of the supercontinuum source is based
on a high peak power femtosecond mode-locked fiber laser. The laser radiates in the spectral
range of the opto-communication wavelengths of 1550 nm, where optical technology is well-
developed. The emitted laser pulses (50 MHz repetition rate) are amplified by an Er-doped
fiber amplifier and launched into a nonlinear fiber that transfers the pulse energy to the 1.9 µm
spectral range, corresponding to the zero-dispersion wavelength of the designed fluoride fiber.
The second amplification stage implies a boost of the optical power in the spectral range of around
2 µm (to >0.5 W average power levels) using the following forward-direction Thulium-doped
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5226

The system presented in Fig. 1 exemplifies the spectacular phenomena of supercontinuum

generation—how a relatively narrow, high-power near-IR laser line is being converted to an
ultra-broadband and bright near- and mid-IR output. Although the schemes, fiber types and design
(for instance, small variations in core diameter can lead to significant changes in the emission
spectrum due to variations in the dispersion profile [76]), pump parameters (duration, peak
power, wavelength relative to the zero-dispersion point, polarization), number and realization
of amplification stages can vary, the basic principle for modern supercontinuum generation
that involves the pump laser and nonlinear fiber is preserved. In the same manner, typically
high output powers (average power levels typically from 100 mW to watts), high beam qualities
(typically M2 ≤ 1.1) and pulsed nature are also being maintained.
From the perspective of mid-IR spectroscopic instrumentation and applications, high peak
powers provided by mid-IR supercontinuum sources (a typical pulse duration is in the ps and
sub-ns regimes) can significantly enhance detection in pulsed measurement modes, keeping
average powers low and hence reducing the thermal load. Applying fast detection systems and
suitable pulse integrators, such as lock-in amplifiers or boxcar gated averagers, the peak gain
(the ratio of the peak to average powers, confined however by the response time of detector) can
be exploited. It can be noted here that near-IR pure continuous-wave (CW) supercontinuum
realizations have been reported but are not well-established and commercialized due to the
inefficiency of the generation (efficiency of the nonlinear processes is suppressed by the meagre
CW-power), poor broadening, requirements to extremely high average power pumping and
km-long fibers resulting in subsequent challenges [128,129].
Apart from the features coming from the lasing nature, supercontinuum radiation has unique
coherence properties. Supercontinua are generated within the guided mode of an optical fiber
(often single mode)—thereby supercontinuum generators preserve high spatial coherence of
the seed-pump laser resulting in high brightness and laser-like focusing properties [130–133].
However, due to the extreme spectral broadening, the temporal coherence is being decoupled
from the spatial one and undergoes changes during the generation process: supercontinuum
light exhibits typically low temporal coherence (extremely short coherence lengths close to
thermal light sources). Figure 2 is intended to illustrate these points demonstrating the typical
emission spectrum of a commercial system (Leukos InF3 fiber based source) and a corresponding
FTIR interferogram (i.e. field-autocorrelation). The Hilbert transform method was used to
determine the coherence lengths shown in Fig. 2(b). The obtained envelopes were used to
extract the full width at half maximum values; a Gaussian fit was additionally applied to the
interferogram envelope of the supercontinuum source due to the slightly asymmetric structure.
The measurements were performed using a commercial FTIR spectrometer (Bruker Optics,
Vertex 70) with default collection parameters (12 spectra averaged, 4 cm−1 resolution, 1 kHz
mirror frequency). A boxcar integration (Zurich Instruments, UHFLI) was used to demodulate
the signal.
Thus, these specific coherence and spectral peculiarities yield a unique emitter, which is of
great interest in various mid-IR spectroscopy applications. Supercontinua eliminate temporal
interference artifacts and maintain diffraction-limited performance, e.g. in hyperspectral imaging
and microspectroscopy. For these reasons, these sources became of great interest also beyond
mid-IR spectroscopy, for instance, in IR optical coherence tomography [134–138].
In the following section, we address and quantify some supercontinuum emission properties
that are particularly relevant for mid-IR spectroscopic applications. Furthermore, we sum up and
feature application scenarios that have been or can be enhanced by novel mid-IR supercontinuum
laser sources.
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5227

Supercontinuum emission
Interferogram
Envelope

Intensity (a.u) ≈4.8 µm

Intensity (a.u)
≈4.8 µm

Interferogram
Envelope
Gaussian fit Globar emission
4500 4000 3500 3000 2500 2000 −100 −50 0 50 100 −100 −50 0 50 100
Wavenumbers(cm−1) Mirror position (µm) Mirror position (µm)

(a) The mid -IR emission spectrum (2.4 µm edge-pass (b) FTIR interferograms: (left) corresponding to the
filter is used) of Leukos InF3 fiber based supercontinuum emission shown in (a) and (right) for
supercontinuum source (250 kHz repetition rate, the thermal emitter; analysis of autocorrelation
650 mW average output power) functions (using the Hilbert transform) is used to
access the actual coherence lengths

Fig.2.2. Emission
Fig. Emission properties
properties of
of aa commercial
commercialsupercontinuum
supercontinuumemitter:
emitter:(a)(a)thethe mid-IR
mid-IR
emission
emission spectrum
spectrum(atmospheric waterwater
(atmospheric vapour and CO
vapour and
2 lead
CO to
2 the
lead characteristic
to the absorption
characteristic
features) and features)
absorption (b) temporal coherence
and (b) temporalproperties
coherence(the interferogram
properties for the conventional
(the interferogram for the
thermal emitter thermal
conventional is shownemitter
for reference).
is shown for reference).

3. Emission properties of mid-IR supercontinuum sources essential to spectro-

3. Emission properties of mid-IR supercontinuum sources essential to spectro-
scopic applications
scopic applications
3.1. Brightness levels of mid-IR supercontinuum sources
3.1. Brightness levels of mid-IR supercontinuum sources
The definition of the brightness of light sources varies over different fields of science [6], therefore,
The definition
in the following ofcalculations
the brightness andofdiscussions,
light sourceswe varies
employoverthe
different fields
definition of science
most familiar[6],
andtherefore,
specific
in the
to laserfollowing calculations
physics [5]. and discussions,
The spectral brightness Bwe employ
of a giventhesource
definition
is an most familiar
emission and specific
property of the
ν̃
to laserthat
source physics [5]. The
describes spectral radiance
its spectral brightness B𝜈˜ of a given
(alternative namingsource
for is
theanbrightness)
emission property of the
and is defined
source
as that describes
the average opticalits spectral
power radiance
P emitted into(alternative naming for
a certain direction perthe
unitbrightness)
surface area and∂Sis per
defined
unit
as theangle
solid average∂Ωoptical
per unitpower P emitted
spectral line ∂ ν̃:into a certain direction per unit surface area 𝜕𝑆 per unit
solid angle 𝜕Ω per unit spectral line 𝜕 𝜈: ˜
∂ 33P
Bν̃ (ν̃) = 𝜕 P , (1)
˜ = cos θ ∂S ∂Ω ∂ ν̃ ,
B𝜈˜ ( 𝜈) (1)
cos 𝜃 𝜕𝑆 𝜕Ω 𝜕 𝜈˜
where θ is the polar angle between the normal to the surface and the vector that defines the
direction
where 𝜃 isofthe
thepolar
emission.
angleIfbetween
Bν̃ is independent
the normaloftoθ,the thesurface
sourceandcan the
be considered
vector that as isotropic
defines the
and omni-directional—the most
direction of the emission. If B 𝜈˜ typical example here is thermal emitters with their spectral
is independent of 𝜃, the source can be considered as isotropic
brightness
and given by Planck’smost
omni-directional—the law (used
typicalinexample
the following
here calculations).
is thermal emitters with their spectral
Equation (1) can be rewritten for laser beams to simplify calculations. Since for highly
brightness given by Planck’s law (used in the following calculations).
collimated
Equationlaser(1) canbeams the divergence
be rewritten for laserangle θ is extremely
beams to simplifysmall, we can assume
calculations. cos highly
Since for θ ≈ 1.
Further, for a beam with the modal diameter D, the effective modal area is πD2/4, and
collimated laser beams the divergence angle 𝜃 is extremely small, we can assume2 cos 𝜃 ≈the1.
a beam with the modal diameter 2
emission solid angle can be defined [5] as πθ 2 . Thereby, the spectral brightness of laser sources
Further, for 𝐷, the effective modal area is 𝜋𝐷 /4, and the
can be given
emission solidasangle
follows:
can be defined [5] as 𝜋𝜃 . Thereby, the spectral brightness of laser sources
can be given as follows: 4 ∂P
Bν̃ (ν̃) = 4 𝜕P , (2)
˜ = (πDθ)22∂ ν̃ ,
B𝜈˜ ( 𝜈) (2)
(𝜋𝐷𝜃) 𝜕 𝜈˜
where ∂P/∂ ν̃ is the power spectral density (PSD) of the source. Hence, brightness as a function
of wavelength
where 𝜕P/𝜕 𝜈˜ iscan
thebepower
explicitly quantified,
spectral density since
(PSD)PSDs,
of theassource.
well asHence,
beam sizes and divergences
brightness as a functionof
of wavelength can be explicitly quantified, since PSDs, as well as beam sizes and divergences of
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5228

various laser
various laser sources,
sources, areare parameters
parameters that that can
can bebe measured
measured using
using standard
standard techniques
techniques or or provided
provided
by manufacturers.
by manufacturers.
In
In order
order to
to stress
stress the
the significance
significance of of spectral
spectral brightness
brightness for
for mid-IR
mid-IR spectroscopy,
spectroscopy, it it should
should be
be
considered in
considered in relation
relation toto optical
optical instruments.
instruments. The The spectral
spectral brightness
brightness isis conventionally
conventionally expressed
expressed
for wavelengths
for wavelengths in in units
units ofof W·sr
W·sr−1 -1
·cm−2 ·nm−1. .On
-2 ·nm-1
Onthetheother
otherside,
side,the
the optical
optical throughput
throughput of of any
any
mid-IR spectrometer
mid-IR spectrometer (or (or etendue,
etendue, aa function
function of of the
the system
system geometry
geometry and
and optical
optical design,
design, defined
defined by
by
the area
the area of
of the
the entrance
entrance pupil
pupil and
and thethe solid
solid angle
angle formed
formed byby the
the collimating
collimating or or the
the focusing
focusing optics)
optics)
is usually
is usually given
given inin units
units of sr·cm22 [139].
of sr·cm [139]. The The product
product ofof multiplication
multiplication of of these
these characteristics
characteristics of
of
the light
the light source
source and
and spectroscopic
spectroscopic system system is is the
the spectral
spectral power
power that
that the
the certain
certain system
system can
can transmit
transmit
and exploit
and exploit for
for spectroscopic
spectroscopic measurements.
measurements. Therefore, Therefore, well-established
well-established mid-IR
mid-IR spectroscopic
spectroscopic
measurement methods
measurement methods can can still
still be
be essentially
essentially improved
improved by by replacing
replacing aa standard
standard thermal
thermal emitter
emitter
with ultra-bright
with ultra-bright supercontinuum
supercontinuum laser laser emitters.
emitters. ForFor instance,
instance, maximum
maximum interaction
interaction lengths
lengths
can be
can be significantly
significantly extended,
extended, thus
thus lowering
lowering limitslimits of
of detection.
detection. InIn photothermal
photothermal spectroscopy,
spectroscopy,
signals can
signals can bebe significantly
significantly amplified.
amplified.
Figure
Figure 33 provides
provides aa quantitative
quantitative visualization
visualization illustrating
illustrating typical brightness levels
typical brightness levels of super-
of super-
continuum sources
continuum sources operating
operating in in the
the IR IR range,
range, as as well
well as
as the
the brightness
brightness of of gold-standard
gold-standard mid-IR
mid-IR
spectroscopic sources:
spectroscopic sources: external-cavity
external-cavity QCLs QCLs and and thermal
thermal emitters.
emitters.

Silica fiber-based supercontinuum Globar 1200 K EC-QCL3 EC-QCL7

ZBLAN fiber-based supercontinuum Globar 1650 K EC-QCL4 EC-QCL8
InF3 fiber-based supercontinuum EC-QCL1 EC-QCL5 EC-QCL9
Chalcogenide fiber-based supercontinuum EC-QCL2 EC-QCL6 EC-QCL10

Wavelength (µm)
9
0.5 1.0 2.0 4.0 8.0 16.0
10
Spectral brightness (W·sr-1·cm-2·nm-1)

Supercontinuum QCL
107 region
region
105

103

101

10−1
Thermal emitters
10−3 region

10−5
20000 10000 5000 2500 1250 625
Wavenumber (cm-1)

Fig.3.3.Spectral
Fig. Spectralbrightness
brightness of
of most representativelight
most representative lightsources
sourcesininmid-IR
mid-IR spectroscopy
spectroscopy
(commercially
(commercially available systems):
available spectral
systems): brightness
spectral levelslevels
brightness of theof
Globars (thermal
the Globars emitters)
(thermal
areemitters)
determined are determined using Plank’s law; the represented supercontinuum sourcesand
using Plank’s law; the represented supercontinuum sources are standard
notare
extreme power
standard andand
notbandwidth versions;
extreme power and EC-QCL
bandwidth - commercial external-cavity
versions; EC-QCL quantum
- commercial
cascade lasers (typical
external-cavity PSDscascade
quantum and beam parameters
lasers are used);
(typical PSDs the spectral
and beam brightness
parameters levels
are used);
arethe
calculated conventionally for average output power (the peak power advantage
spectral brightness levels are calculated conventionally for average output power discussed
below
(the is not power
peak considered).
advantage discussed below is not considered).

The
The brightness
brightness levels
levels of
of the
the laser
laser sources
sources depicted in Fig.
depicted in Fig. 33 were
were calculated
calculated according to
according to
Eq. (2). The PSDs, as well as the beam parameters of the silica-, InF 3 and chalcogenide-fiber
Eq. (2). The PSDs, as well as the beam parameters of the silica-, InF3 and chalcogenide-fiber
based
based supercontinuum
supercontinuum sources,
sources, were
were provided
provided by
by Leukos.
Leukos. TheThe emission
emission parameters
parameters of
of the
the
ZBLAN-fiber
ZBLAN-fiber based supercontinuum source were provided by NKT Photonics. For the QCL
based supercontinuum source were provided by NKT Photonics. For the QCL
emitters
emitters typical
typicalemission
emissionproperties
propertiesof of
commercial systems
commercial (DRS
systems Daylight
(DRS Solutions)
Daylight were used;
Solutions) were
used; the CW operation mode was considered as it provides the narrowest spectral linewidth of
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5229

the CW operation mode was considered as it provides the narrowest spectral linewidth of 100
MHz.
Spectral brightness, as an explicit application-oriented metric to compare mid-IR emitters,
clearly shows that ultra-broadband supercontinuum laser sources effectively fill the gap between
thermal sources and QCLs. Thermal emitters are broadband but feature low brightness emission,
while high-brightness QCL sources are relatively limited in spectral coverage, in particular, for
the single laser ridge configuration. Thus, supercontinuum sources provide laser-like spectral
brightness levels while maintaining an instantaneous ultra-broadband spectral coverage (close to
thermal emitters in this sense) for each sub-ns pulse.
Considering the pulsed nature of the supercontinuum emission, another point has to be
emphasized again in this context. The spectral brightness levels depicted in Fig. 3 are calculated
for average powers that mostly heat the sample (typical PSD levels in µW - mW ranges per
nm-line) and not for the peak power levels. In the typical supercontinuum short-pulse emission
regime, peak power levels can reach several watts within the same nanometer spectral band
and thus peak brightness can be significantly higher. The conventional definition used above is
completely valid for slow IR detectors. Nevertheless, fast semiconductor detectors (e.g. HgCdTe,
InSb and InAsSb) can exhibit sub-ns rise time [140], thus, coupled to a suitable detection system
(e.g. boxcar integrators) the peak power signal advantage can be gained. Hence, applying a
proper detection scheme, pulsed supercontinuum sources can reach comparable brightness levels
as for instance QCL lasers or even surpass them.

3.2. Beam quality

Emission features that significantly distinguish supercontinuum laser sources from standard
emitters used in applied mid-IR spectroscopy—from both thermal and laser sources—are
high beam quality and spatial stability. Thus, unlike, for example, QCL technology, mid-IR
supercontinua generated in optical fibers have superior characteristics in terms of beam profile,
divergence (beam qualities are severely limited for QCLs [141,142]), and beam symmetry
(no astigmatism, common for QCL emission [13,141,142]). Besides, supercontinuum sources
provide an intrinsic mode-hop free operation.
The beam quality practically reflects the quality of the evolution of energy spatial distribution
along the propagation direction. It not only directly affects the spectral brightness of the laser

Measured caustic Hyperbolic fit Rayleigh ranges Divergence angle

w0 = d0 /2=279±1µm, M 2 = 1.09±0.00, λ=4000 nm
-4zR -3zR -2zR -zR 0 zR 2zR 3zR 4zR

1000
1/e2 beam size (µm)

500

0 Θ = 9.93±0.01 mrad

−500

−1000 z < −2zR −zR < z < zR 2zR < z

-225 -169 -112 -56 0 56 112 169 225

Axial location (mm)

4. Characterization
Fig. Fig. 4. Characterization of the M2Mbeam
of the 2 beam quality
qualityfactor
factorwithin
withinthe
themid-IR
mid-IRsub-band
sub-band (M
2
≈ 1.09,
(M2500 nm 500
≈ 1.09, band,
nm4 band,
µm center wavelength)
4 µm center for afor
wavelength) commercial
a commercialmid-IR ZBLAN-based
mid-IR ZBLAN-
supercontinuum source (NKT
based supercontinuum sourcePhotonics); the complete
(NKT Photonics); recorded
the complete 3-dimensional
recorded 3-dimensionalbeam
evolution
beam(in pseudo(in
evolution colors)
pseudo is shown
colors)inisthe background
shown for reference
in the background for (radial asymmetry
reference (radial is
due to the spherical
asymmetry mirror
is due to thethat was used
spherical to avoid
mirror oversaturation);
that was used to avoidthe analysis is performed
oversaturation); the
for the meridional
analysis plane (the
is performed input
for the beam profile
meridional planeis(the
Gaussian).
input beam profile is Gaussian).

In most applied cases, a practical parameter that characterizes and quantifies the laser beam
quality sufficiently well is the M2 factor [5]. It essentially indicates how strongly the actual beam
differs from the theoretical diffraction-limited one (diffraction-limited Gaussian beam has an M2
factor of 1). The beam quality factor has an explicit practical meaning so that the resolution of,
for example, any hyperspectral aberration-free microscope that employs the mapping approach
can be estimated by multiplying the theoretical diffraction-limited resolution with the M2 factor
of the exploited light source [143].
2
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5230

Gaussian
30000 (a) 30000 (b) Gaussian

Intensity

Intensity
20000 20000

10000 10000
dx=582 µm dy=2445 µm

0 0
−500 0 500 −2000 −1000 0 1000 2000
Distance from center (µm) Distance from center (µm)
Distance from center (µm)

6
(c) (d)
1000

Y coordinate (mm)
4
0

2
−1000

−2000 0 2000 0
1 0 1
Distance from center (µm)
0
0 2 4 6
X coordinate (mm)

Fig. 5.5.Profiles
Fig. ofof
Profiles thethe
mid-IR
mid-IR supercontinuum
supercontinuum beam
beamobtained
obtainedfrom M2Mcharacterization
thethe
from 2 characteri-
(4 zation
µm center wavelength,
(4 µm 500 nm bandwidth)
center wavelength, at different
500 nm bandwidth) at positions: (a-c) close(a-c)
different positions: to the focus
close
position
to the (a,b
focusare for major
position (a,band
areminor axesand
for major of the on-purpose
minor astigmated
axes of the beam);
on-purpose (d) actual
astigmated
outgoing
beam); beam of the
(d) actual supercontinuum
outgoing beam of thelaser source measured
supercontinuum laserdirectly after the collimator
source measured directly
(normalized, the bolometer is not field corrected).
after the collimator (normalized, the bolometer is not field corrected).

The supercontinuum
source through the divergence beam caustic
and modal has been
area, recorded with an axial
but also determines thestep of 1 mm.
focusing Figure 4
performance.
depicts the results of the measurements and characterization of the M 2 (all the points within the
Thus, this emission feature removes the trade-off between spatial and spectral performance 2 factor is
[−𝑧 𝑅 < 𝑧for
inherent 𝑅 ] and [𝑧
< 𝑧thermal < −2𝑧 𝑅and
emitters ] ranges
becomeswereofused for calculation).
particular interest forThee.g.resulting
remote M sensing and
1.09, due spectroscopic
stand-off to a large number of measurement
applications, chemicalpoints,
imagingthe uncertainty
and mapping, is inand
the microspectroscopy.
thousandths (0.0035).
TheInpostprocessing
most applied cases, of theameasurements
practical was performed
parameter using theand
that characterizes freequantifies
Python library [145].
the laser beam
Figure 5 supplements the M 2 characterization and displays a beam profile (with corresponding
2
quality sufficiently well is the M factor [5]. It essentially indicates how strongly the actual beam
Gaussian
differs fromfitsthefortheoretical
the semi-major and semi-minor
diffraction-limited oneaxes) taken from the Gaussian
(diffraction-limited recorded caustics
beam hasclose
an Mto2
the focus position [see Fig. 5(a-c)]. A normalized polychromatic beam
factor of 1). The beam quality factor has an explicit practical meaning so that the resolution of, profile captured before
the example,
for focusing system is shown inaberration-free
any hyperspectral Fig. 5(c). microscope that employs the mapping approach
can be estimated
3.3. Long-term stabilityby multiplying the theoretical diffraction-limited resolution with the M2 factor
of the exploited light source [143].
A procedure
Besides for determining
the laser-like emission the M2 factormodern
properties, is defined by the
mid-IR ISO Standard 11146
supercontinuum sources[144]. It
feature
involves
sufficientthe measurement
long-term of thestability
intensity beam caustic (for6)atthat
(see Fig. leastenables
five beam locationsinwithin
flexibility one Rayleigh
measurements and
distance
integration [zRwithout
] and fiverecalibration
locations at of distances more than
spectroscopic two Rayleigh lengths from the waist) from
instruments.
which the M2 stability
Long-term can be calculated analyzing the
can be characterized evolution
in several ways.of the
Thebeam
most radius accessed method
straightforward using theis
D4σ second
to assess the moment
stability ofof the
the intensity
emission distribution
power over amethod.reasonably long period of time. Figure 6(a)
In this
depicts thesection, we provide
time-evolution of thethe
outputM2 average
characterization
power for aforcommercial
a typical mid-IR ZBLAN-based
mid-IR supercontinuum
supercontinuum source (NKT Photonics, SuperK Compact, 40 mW output
laser source (Novae, Coverage, 2.4 MHz repetition rate, spectral coverage approx. 5200 cm-1
frompower).
to In -1 ). The measurements were performed using a mid-IR compatible power meter
order
2380 cmto access the beam quality of the mid-IR supercontinuum emission, an all-mirror
focusing optical arrangement
(Coherent, LabMax TOP Power (toMeter,
eliminate
LM-10 chromatic aberration)
HTD detector head)was seta up:
with a 750
sample mmstep
time focal
of
length gold spherical mirror was used. The spectral range was limited using a suitable band-pass
3 min. The relative output power fluctuations were 0.2%, however, it should be noted that the first
spectral
period offilter
around (center wavelength
20 min is 4 µm or
caused stronger 2500 cmas−1the
variations , 500 nm bandwidth,
source showed a drift Thorlabs
in theFB4000-
average
500). The beam profiles at different positions were recorded using a bolometer array (FLIR
output power during this warm-up time (excluding this time-span, the relative fluctuations are
Boson, 640x480 px) fixed on a 20 cm scanning stage; the scanning range covers the necessary
below 0.15%).
Rayleigh
In orderdistances
to evaluate according to the ISO
the long-term standard
stability 11146.
in terms of integration performances (i.e. to access
the limits of averaging), distinguish potential noise sources and types of intensity fluctuations, an
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5231

Stability: 99.8% Stability: 99.81%

Power (mW)
231
0.92 230
229

0.90 20 40 60

Average power (W)

Measurement time (h)

White noise
0.88

Allan Variance σA2

10−6

Optimal
0.86 integration
time

ifts
Dr
0.84
10−7

0 100 200 300 400 500 102 103 104 105

Measurement ime (min) Integration time (s)

(a) Output power of a ZBLAN-based (b) Allan variance plot (bottom) for the
supercontinuum source (Novae, Coverage), output intensity of a ZBLAN-based mid-IR
recorded over 500 min (3 min sampling supercontinuum source (NKT Photonics,
period); the mean value is 875 mW, the SuperK mid-IR); calculated for the series of
standard deviation is 1.7 mW the recorded power levels (top);

Fig.6.6. Long-term
Fig. stability of
Long-term stability ofthe
themid-IR
mid-IRsupercontinuum
supercontinuumsources
sources characterized
characterized forfor
commercial
commercial systems in the
systems formform
in the of (a)ofthe
(a)power stability
the power (Novae(Novae
stability supercontinuum emitter, 8
supercontinuum
h)emitter,
and (b) 8the
h)Allan variance
and (b) (NKT
the Allan photonics,
variance (NKT65photonics,
h). 65 h).

The supercontinuum beam caustic has been recorded with an axial step of 1 mm. Figure 4
depicts themeasure
alternative results ofcan
thebemeasurements
employed. Inand characterization
spectroscopic of the M2the
measurements, (alllimit
the points withinisthe
of detection a
[−zR <z<zR ] and [z< − 2zR ] ranges were used for calculation). The resulting M factor is 1.09,
function of the integration time coupled with the long-term stability of the 2
instrument (i.e. mean
due to from
values a largeannumber
averagingof measurement points,
process are being the uncertainty
recorded, is in the
for instance, thousandths
using e.g. pulse(0.0035).
averagingTheor
postprocessing of the measurements was performed using the free Python library [145].
interferogram averaging). Thus, the concept of Allan variance [146, 147] that is in essence the
Figure 5 supplements
two-sample variance of the M2 characterization
the data cluster averagesandas adisplays
functiona beam profile
of cluster (with corresponding
size—first adopted for
Gaussian fits for the semi-major and semi-minor axes) taken from the recorded caustics closethe
spectroscopy by Werle [148, 149]—can be used. In the following assessment, we employed to
the focus position
overlapping [see Fig. estimator
Allan variance 5(a-c)]. Athat,
normalized polychromatic
in contrast to the standard beam profile
Allan captured
variance before
algorithm
the focusing
used by Werle,system is shown
exploits in Fig.
all possible 5(c).
combinations for the given data set by introducing overlapping
clusters, and hence exhibits higher confidence [150, 151]. The following Allan variance estimator
3.3.used:
was Long-term stability
𝑁∑︁
−2𝑘
1
Besides the laser-like𝜎emission
2 properties,
𝐴 (𝑘 · 𝜏0 , 𝑁) =
modern mid-IR supercontinuum
[ 𝐴 𝑗+𝑘 − 𝐴 𝑗 ]2, sources feature
(3)
sufficient long-term intensity stability 2(𝑁 − 2𝑘6)
(see Fig. + that
1) 𝑗=0
enables flexibility in measurements and
integration without recalibration of spectroscopic instruments.
where 𝐴 𝑗 is the average value of the jth cluster (also known as subgroups), 𝑘 is the cluster size
Long-term stability can be characterized in several ways. The most straightforward method is
(number of elements in the cluster), 𝜏0 · 𝑘 is the observation time (𝜏 = 𝜏0 · 𝑘, 𝜏0 is the sampling
to assess the stability of the emission power over a reasonably long period of time. Figure 6(a)
period), 𝑁 is the total number of samples, the same notation as in [148] is used here for simplicity.
depicts the time-evolution of the output average power for a commercial mid-IR supercontinuum
The average value of the jth cluster is calculated then as:
laser source (Novae, Coverage, 2.4 MHz repetition rate, spectral coverage from approx. 5200
cm−1 to 2380 cm−1 ). The measurements were performed using a mid-IR compatible power meter
1 ∑︁
𝑗+𝑘
(Coherent, LabMax TOP Power Meter, LM-10 𝐴𝑗 = HTD detector
𝑥𝑖 , head) with a sample time step of (4)3
min. The relative output power fluctuations were 𝑘 𝑖=0.2%,
𝑗 however, it should be noted that the first
period of around 20 min caused stronger variations as the source showed a drift in the average
output𝑥power
where 𝑖 is theduring this warm-up
ith element time
of the data set.(excluding this time-span, the relative fluctuations are
below 0.15%).
Hence, the average output power sampled over a long period of time is chosen for the analysis
In order
here. It has to
to evaluate
be noted,the long-term
that stability
this property wasinselected
terms ofsinceintegration performances
the source fluctuations(i.e.
aretoisolated
access
the limits
and of averaging),
the resulting distinguish
Allan variances potential
can noise sources
be considered and types of of
as a characteristic intensity fluctuations,
the source. Thus, the an
alternative
Allan measure
variance plot can be employed.
expresses In behavior
the noise spectroscopic
of themeasurements,
supercontinuum the limit ofin
source detection
a long runis a
function of of
(regardless thethe
integration time
initial time coupledand
moment) withdefines
the long-term
average stability of the instrument
optimal integration times (i.e. mean
and noise
reduction capabilities.
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5232

values from an averaging process are being recorded, for instance, using e.g. pulse averaging or
interferogram averaging). Thus, the concept of Allan variance [146,147] that is in essence the
two-sample variance of the data cluster averages as a function of cluster size—first adopted for
spectroscopy by Werle [148,149]—can be used. In the following assessment, we employed the
overlapping Allan variance estimator that, in contrast to the standard Allan variance algorithm
used by Werle, exploits all possible combinations for the given data set by introducing overlapping
clusters, and hence exhibits higher confidence [150,151]. The following Allan variance estimator
was used:
1 ∑︂
N−2k
σA2 (k · τ0 , N) = [Aj+k − Aj ]2 , (3)
2(N − 2k + 1) j=0

where Aj is the average value of the jth cluster (also known as subgroups), k is the cluster size
(number of elements in the cluster), τ0 · k is the observation time (τ = τ0 · k, τ0 is the sampling
period), N is the total number of samples, the same notation as in [148] is used here for simplicity.
The average value of the jth cluster is calculated then as:

1 ∑︂
j+k
Aj = xi , (4)
k i=j

where xi is the ith element of the data set.

Hence, the average output power sampled over a long period of time is chosen for the analysis
here. It has to be noted, that this property was selected since the source fluctuations are isolated
and the resulting Allan variances can be considered as a characteristic of the source. Thus, the
Allan variance plot expresses the noise behavior of the supercontinuum source in a long run
(regardless of the initial time moment) and defines average optimal integration times and noise
reduction capabilities.
Figure 6(b) depicts the Allan plot for a ZBLAN-based mid-IR supercontinuum source (NKT
Photonics, SuperK mid-IR, spectral coverage from approx. 6600 cm−1 to 2250 cm−1 , around
230 mW of mid-IR power, anomalous pump scheme). The variance was derived for a series
of average power measurements, the sampling period was 30 sec, total evaluation time was 65
hours. The obtained Allan plot reveals that at low integration times, white noise dominates as the
variance decreases proportionally to the averaging time. The origin of the observed white noise
can be attributed to the characteristic property of the supercontinuum generation with pumping
in the anomalous mode [82,95]. The Allan plot also shows that the signal-to-noise ratio can be
improved by more than one order of magnitude by averaging over the optimal time period. The
observed long-term fluctuations start to contribute negatively beyond the optimal integration time
of around 1500 sec reducing integration efficiency. A second noise reduction can be observed for
a cluster size larger than one day (non-expedient times for single spectroscopic measurements).
These daily fluctuations can be correlated with e.g. temperatures changes.

3.4. Spectral stability

The presented long-term measurements reflect the time-stability of the average power of the
supercontinuum sources and thus signal-to-noise enhancements achievable by increasing the
measurement time. However, another metric that is of high interest for mid-IR spectroscopy is
emitter-induced spectral fluctuations on time intervals on the scale of a standard measurement
time. From this point of view, zero absorbance lines provide an insight into this property.
They are calculated as Beer’s absorbance for two sequentially measured spectra under the
same conditions with no changes in the optical path and system. Thereby, they can be used
to evaluate noises of different emitters as they show wavenumber-dependent instabilities. We
performed these measurements with no sample inserted. Intensities were artificially scaled to
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5233

comparable levels using neutral-density filters and different aperture sizes. Hence, the results do
not represent the merit of the absolute signal-to-noise ratio available: e.g. by increasing path
lengths for spectroscopic measurements, signals for thermal sources can be strongly or completely
suppressed, while supercontinua can still efficiently penetrate. Quantitative assessments of
spectral noise for various state-of-the-art laser-based mid-IR spectroscopic methods can be found
in [152].
In order to characterize the spectral performance of mid-IR supercontinuum sources and
to compare them to a standard thermal emitter, excluding possible contributions from the
instrumental noise, we used a commercial FTIR spectrometer (Bruker Optics, Vertex 70) as
the core system and a mid-IR detector (Mercury Cadmium √ Telluride variable gap detector,
MCT, Vigo PCI-4TE-12, detectivity D = 2.0 × 109 cm · Hz · W−1 ) for all characterization
measurements. The acquisition parameters and settings of the spectrometer and detector were
fixed, so the measurement time for noise estimation was set constant (around 5 sec per spectrum)
for different sources. Figure 7 depicts the zero absorbance lines measured for three mid-IR
supercontinuum sources and for the built-in FTIR Globar respectively.
Since supercontinuum sources are pulsed low-duty cycle light emitters, a boxcar integrator
(gated integrator, Zurich Instruments, UHFLI) was used to demodulate and pre-process the signal
for acquisition by the read-out electronics of the spectrometer. Therefore, the inter-pulse noise
was excluded by averaging the signal during an optimally configured time gate (from 20 to 50
ns). This type of integrator was selected as it is more efficient for non-sinusoidal low-duty cycle
sources compared to lock-in amplifiers [153]. We assumed that the integrator does not introduce
significant noise, allowing to compare the pulsed supercontinua with the CW thermal emission.
All the measurements shown in Fig. 7 were performed with a locked configuration and
parameters of the spectrometer. An edge-pass filter (2.4 µm cut-on wavelength) was used to
select the mid-IR spectral band. In order to operate the detector close to the saturation regime,
the size of the aperture was adjusted due to the different brightness levels of the light sources.
Since one of the supercontinuum lasers (Leukos, InF3 fiber based) has considerably higher pulse
energy (650 mW average power, 250 kHz repetition rate) compared to the other sources, a strong
neutral density filter was employed to scale the emission of the former (1% transmission, Thorlabs
NDIR20B, spectral intensity noise is assumed to be scaled proportionally). The mirror frequency
of the FTIR system was fixed at 1 kHz for the characterization, thus, the measurement time
window was constant for noise evaluation. Depending on the pulse repetition rate of the source,
the boxcar integrator (i.e. an interferogram demodulation device) was configured individually in
order to avoid a smear out of the high frequency components in the respective interferograms.
This smear out is caused due to the high mirror velocity relative to the effective bandwidth of
the boxcar integrator. The boxcar time constant was set to 1024 cycles (equivalent to 410 µs
time constant) for the supercontinuum source from NKT Photonics, to 128 cycles (512 µs time
constant) for the supercontinuum laser from Leukos, and to 32768 cycles (655 µs time constant)
for Thorlabs SC4500. The obtained spectra were smooth owing to the high signal-to-noise ratio.
Considering the results of the characterization depicted in Fig. 7 and the obtained RMS errors,
it has to be noted that the high repetition rate supercontinuum generators from NKT Photonics
and Thorlabs possess the superior spectral stability (spectral deviations cannot be distinguished
by eye), and in the small ranges they surpassed the thermal emitter in the given configuration.
However, the spectral noise performance of the ZBLAN supercontinuum-based FTIR can still
be improved by flattening the spectral shape or removing the intense spectral peak to efficiently
exploit the dynamic range of the detector and DAQ unit, which can result in comparable noise
levels in relatively broad spectral ranges.
All the characterized supercontinuum sources are conventional, based on an anomalous
dispersion generation scheme. Figure 7 confirms and illustrates the commonly known fact
that supercontinuum sources employing pumping in the anomalous dispersion regime exhibit
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5234

0.10 0.10

Absorbance (abs.u.)

Absorbance (abs.u.)
0.05 0.05

0.00 0.00

−0.05 −0.05

−0.10 −0.10
Power spectrum (a.u.)

Power spectrum (a.u.)

0.2
1.0

0.1
0.5

0.0 0.0
4500 4000 3500 3000 2500 2000 4500 4000 3500 3000 2500 2000
Wavenumbers(cm−1) Wavenumbers(cm−1)

(a) Leukos InF3 fiber based supercontinuum source (b) NKT photonics ZBLAN fiber based
(600 mW, 250 KHz; 1% ND filter used); supercontinuum source (500 mW, 2.5 MHz);
RMS=0.0065 (abs.u.) RMS=0.0025 (abs.u.)
0.10 0.10

Absorbance (abs.u.)
Absorbance (abs.u.)

0.05 0.05

0.00 0.00

−0.05 −0.05

−0.10 −0.10
Power spectrum (a.u.)
Power spectrum (a.u.)

0.10
0.04

0.05 0.02

0.00 0
4500 4000 3500 3000 2500 2000 4500 4000 3500 3000 2500 2000
Wavenumbers(cm−1) Wavenumbers(cm−1)

(c) Thorlabs SC4500 InF3 fiber based (d) Standard on-board thermal emitter;
supercontinuum source (300 mW, 50 MHz); RMS=0.0012 (abs.u.)
RMS=0.0024 (abs.u.)

7. Zero
Fig. Fig. absorbance
7. Zero absorbancelines measured
lines measured using a standard
using a standardFTIR
FTIRinstrument
instrumentemploying
employing(a-c)
mid-IR
(a-c)supercontinuum sourcessources
mid-IR supercontinuum and (d)anda conventional thermal
(d) a conventional emitter;
thermal emission
emitter; emissionpower
spectra are spectra
power shown below in corresponding
are shown sub-plots sub-plots
below in corresponding for reference (characteristic
for reference absorptions
(characteristic
of atmospheric
absorptions CO 2 and H2 O are 2present),
of atmospheric CO and H2 Odetector dark detector
are present), noise floordarkisnoise
3.3×10 −5 is(a.u);
floor
-5 (a.u); the
the FTIR spectrometer, detector (MCT) and their parameters were set the same set
3.3×10 FTIR spectrometer, detector (MCT) and their parameters were for all
measurements,
the same forthus, the measurement
all measurements, thus,time for noise evaluation
the measurement was set
time for noise constantwas
evaluation (around
set 5
constant
sec per (around
spectrum); the5mid-IR
sec per part
spectrum); the mid-IRwas
of the spectrum partselected
of the spectrum wasµm
using a 2.4 selected
edge-pass
using a 2.4 µm edge-pass spectral filter; the RMS errors are calculated for the spectral−1
spectral filter; the RMS errors -1are calculated-1for the spectral-1bandwidth from 4025 cm to
bandwidth from 4025 cm to 2280 cm [to 2500 cm for (c) due to the limited
2280 cm−1 [to 2500 cm−1 for (c) due to the limited coverage].
coverage].

relatively high fluctuations (especially in comparison to the novel concept of all-normal dispersion
Since supercontinuum sources are pulsed low-duty cycle light emitters, a boxcar integrator
supercontinuum generators [42,95,154,155]). However, the figure also shows the importance
(gated integrator, Zurich Instruments, UHFLI) was used to demodulate and pre-process the signal
of pulse averaging, so that high pulse repetition rate emitters (in MHz or tens MHz range) can
for acquisition by the read-out electronics of the spectrometer. Therefore, the inter-pulse noise
diminish the effects of pulse-to-pulse spectral instabilities for most routine mid-IR spectroscopic
was excluded by averaging the signal during an optimally configured time gate (from 20 to 50 ns).
applications.
This type ofAnintegrator
illustrative
wasexample
selectedforasnoise reduction
it is more by integration
efficient using high
for non-sinusoidal repetition
low-duty rates
cycle
in the
sources compared to lock-in amplifiers [153]. We assumed that the integrator does not introducebe
extreme noise sensitive technique of spectral-domain optical coherence tomography can
found in [156].
significant Moreover,
noise, allowingwetowould likethe
compare to pulsed
point out that the enhancement
supercontinua with the CWin thermal
spectralemission.
brightness
enables to significantly extend light-matter interaction path lengths and to probe more molecules
(i.e. intensifying absorbance signals with respect to noise). Thus, the relatively higher spectral
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5235

instabilities (in the standard measurement time scale) of supercontinuum sources compared to
standard thermal emitters become insignificant in practice.
Additionally, we extend the concept of the Allan variance defined in the previous section and
apply it to visualize the presence of spectrally dependent drifts for the FTIR-based instrument (see
Fig. 8). It should be noted, however, that the resulting 2-dimensional Allan variance should not
be considered as an absolute assessment for the emitter stability (i.e. for evaluation of absolute
optimal integration time), but rather as a relative one (illustrating relative behavior of constituent
spectral components). Contributions from other sub-systems (such as detector instabilities, drifts
of the power supplies, temperature-induced variations, deviations in the spectrometer parameters
etc.) are superimposed on the drifts of the mid-IR supercontinuum laser source itself. For
instance, strong and sharp changes in the integral of the recorded emission spectra were observed
in the mornings due to changes in the building’s electrical power supply, although, these changes
are not visible in the average power stability characterization of the emission (i.e. more isolated
source characterizations).
source characterizations). Therefore,
Therefore, we
we neglected
neglected thethe above-mentioned
above-mentioned non-emission
non-emission related
related
drifts and
drifts and calculated
calculated the
the Allan
Allan variance
variance for
for aa 12
12 hour
hour time
time period
period where
where those
those drifts
drifts did
did not
not occur
occur
(i.e. source
(i.e. source related
related drifts
drifts presumably
presumably dominate).
dominate). Hence,
Hence, any
any spectral
spectral instability
instability for
for this
this time
time
period can
period can be
be accounted
accounted toto be
be aa property
property of
of the
the analyzed
analyzed laser
laser and
and not
not of
of the
the aforementioned
aforementioned
external sources.
external sources. Thus,
Thus, the
the practical
practical reasoning
reasoning behind
behind this
this analysis
analysis to
to distinguish
distinguish the
the relative
relative
time-stability of
time-stability of the
the different
different spectral
spectral regions
regions ofof the
the supercontinuum
supercontinuum emission
emission isis valid.
valid.

σA2
10−3

4000

3750
10−4
Wavenumbers (cm−1)

3500

3250
10−5

3000

2750
10−6

2500

2250
10−7
102 103 104
Integration time (s)

Fig. 8. Spectral 2-dimensional Allan variance for the emission of the mid-IR supercontinuum
Fig. 8. Spectral 2-dimensional Allan variance for the emission of the mid-IR super-
source (NKT Photonics, SuperK mid-IR) visualizing relative spectral drifts (an FTIR
continuum source (NKT Photonics, SuperK mid-IR) visualizing relative spectral drifts
instrument was used for evaluation); this is a source-specific characterization measurement
(an FTIR instrument was used for evaluation); this is a source-specific characterization
showing the spectral dependent stability and drifts; for small cluster sizes it correlates with
measurement showing the spectral dependent stability and drifts; for small cluster sizes
zero absorbance lines but provides additional insights into temporal behavior; the emission
it correlates with zero absorbance lines but provides additional insights into temporal
spectrum is shown for reference as the black overlay.
behavior; the emission spectrum is shown for reference as the black overlay.

The intensity of various spectral components were analyzed over the time interval of 12 hours,
The intensity of various spectral components were analyzed over the time interval of 12 hours,
which is also a reasonable time-span for single-day measurements. The sampling period for
which is also a reasonable time-span for single-day measurements. The sampling period for
the emission spectra was around 100 sec, the spectral resolution was set to 4 cm−1 . Figure 8
the emission spectra was around 100 sec, the spectral resolution was set to 4 cm-1 . Figure 8
depicts the resulting 2-dimensional Allan variance. It can be noted that the initial shape (i.e.
depicts the resulting 2-dimensional Allan variance. It can be noted that the initial shape (i.e.
the variance for single-measurement clusters) of the spectral Allan variance correlates with the
the variance for single-measurement clusters) of the spectral Allan variance correlates with the
zero absorbance lines shown in Fig. 7(b). However, in contrast to zero-absorbance lines, which
zero absorbance lines shown in Fig. 7(b). However, in contrast to zero-absorbance lines, which
always characterize the deviation between two subsequent spectra (only short-time changes can
always characterize the deviation between two subsequent spectra (only short-time changes can
be detected), the Allan variance provides the assessments for statistically average spectral stability
across the entire time interval, regardless of the initial time point.
Analyzing the Allan plot shown in Fig. 8, several pronounced features can be distinguished.
For instance, the broad and strong spectral peak centered at around 2400 cm-1 , which appeared
to be highly stable in the short run (superior to the thermal emitter, as also demonstrated by
zero absorbance lines), exhibits the presence of relatively stronger intensity drifts and, therefore,
lower integration capabilities than other spectral sub-bands (the optimal integration time here is
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5236

be detected), the Allan variance provides the assessments for statistically average spectral stability
across the entire time interval, regardless of the initial time point.
Analyzing the Allan plot shown in Fig. 8, several pronounced features can be distinguished.
For instance, the broad and strong spectral peak centered at around 2400 cm−1 , which appeared
to be highly stable in the short run (superior to the thermal emitter, as also demonstrated by
zero absorbance lines), exhibits the presence of relatively stronger intensity drifts and, therefore,
lower integration capabilities than other spectral sub-bands (the optimal integration time here is
below 1000 sec). For the rest of the spectrum, the slope characteristic for white noise dominates
until reaching the minimum of Allan variance. The mean optimal averaging time is in the
range of around 1500 sec, which is in agreement with the measurements shown in the previous
section [Fig. 6(b)]. Furthermore, for some spectral regions a noise reduction after 104 sec can
be observed. These facts confirm our assumptions that the selected time interval of 12 hours is
suitable
suitable for
for the
the analysis
analysis of
of the
the emission
emission stability.
stability. A
A particularly
particularly interesting
interesting spectral
spectral behavior,
behavior, i.e.,
i.e.,
an
an increased
increased long-term
long-term stability
stability of
of the
the spectral
spectral shape
shape with
with aa predominance
predominance of of white
white noise,
noise, can
can
be
be also
also observed
observed inin the
the range
range between
between approximately
approximately30003000cmcm−1-1 and
and 3250
3250 cm . This spectral
-1 . This spectral
cm−1
window
window (especially
(especially around
around 3100 µm) is
3100 µm) is quite
quite important
important for
for mid-IR
mid-IR spectroscopy
spectroscopy due
due to
to the
the
presence
presence ofof distinct
distinct absorption
absorption bands
bands (stretching
(stretching vibrations
vibrations of
of the
the C-H,
C-H, N-H,
N-H, O-H
O-H groups).
groups).

3.5. Summary of
of the properties
properties andand their
their relation
relation to specific
to specific spectroscopic
spectroscopic applications
applications
The
The purpose
purpose of of this
this section
section is
is to
to generalize
generalize thethe most
most important
important and,
and, atat the
the same
same time,
time, the
the most
most
distinctive
distinctive properties
properties ofof supercontinuum
supercontinuum laser laser sources
sources relevant
relevant for
for applied
applied mid-IR
mid-IR spectroscopy.
spectroscopy.
Therefore,
Therefore, we we conclude
conclude this
this part
part by
by summarizing
summarizing and and listing
listing the
the characteristic
characteristic parameters
parameters andand
identifying
identifying potential
potential applications
applications that
that promise
promise to to be
be or
or have
have already
already been
been advanced
advanced byby mid-IR
mid-IR
supercontinuum
supercontinuum technology.
technology.
The brief summary of
The brief summary of the
the key
key properties
properties andand their
their relation
relation to
to certain
certain applied
applied scenarios,
scenarios, inin
which they are expected to have the strongest impact, is given in Fig. 9. Here we once again
which they are expected to have the strongest impact, is given in Fig. 9. Here we once again
emphasize
emphasize the the importance
importance of of laser-like
laser-like emission
emission properties
properties ofof supercontinua
supercontinua (beam
(beam quality,
quality,
spatial coherence, uni-directionality) coupled with the high spectral brightness, stability, and
spatial coherence, uni-directionality) coupled with the high spectral brightness, stability, and
ultra-broadband spectral coverage. The mid-IR supercontinuum technology can provide instant
ultra-broadband spectral coverage. The mid-IR supercontinuum technology can provide instant
access
access to
to the
the functional
functional group
group asas well
well asas the
the fingerprint
fingerprint area
area with
with aa single
single emitter.
emitter. Thus,
Thus, such
such aa
combination of emission properties is unique and non-specific to any other mid-IR laser source.
combination of emission properties is unique and non-specific to any other mid-IR laser source.
Hence,
Hence, the
the strict
strict categorization
categorization given
given here
here is
is simplified
simplified to to show
show the
the most
most striking
striking implications.
implications.
Discussion of the specific properties of supercontinuum radiation (no mid-IR supercontinuum
Discussion of the specific properties of supercontinuum radiation (no mid-IR supercontinuum
considered
considered at at this
this point)
point) and
and their
their relation
relation toto spectroscopic
spectroscopic application
application scenarios
scenarios can
can also
also be
be
found in [157].
found in [157].

Compact and stable design (OEM Straightforward integration into

solutions available); room tempe- existing systems; operation
rature operation; fiber output under standard conditions;

Supercontinuum High spectral brightness; Absorption spectroscopy (long

sources in the ultra-broadband flat emission; path lengths); multimodality;
mid-IR spectral long and short term stability photothermal approaches
range
Laser emission properties (diffrac- Hyperspectral imaging,
tion-limited beam quality,uni- microspectroscopy, chemical
directionality, spatial coherence) mapping; stand-off spectoscopy;

Adjustable pulse duration, repe- Sensitivity enhanced absorption

tition rate; high peak power; measurements (peak brightness);
laser-like emission properties photothermal spectroscopy

Fig. 9. 9.Brief
Fig. Briefsummary
summaryof the characteristic
of the features
characteristic of mid-IR
features supercontinuum
of mid-IR laser sources;
supercontinuum laser
highlighted according toaccording
sources; highlighted potential to
applied cases
potential and scenarios.
applied cases and scenarios.

In the following section, we supplement the scheme reviewing the current state-of-the-art and
providing up-to-date achievements in the distinguished fields.

4. Supercontinuum sources in mid-IR spectroscopy: an overview of state-of-the-

art applications
Supercontinuum laser sources have been used for applied IR spectroscopy (primarily near-IR)
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5237

In the following section, we supplement the scheme reviewing the current state-of-the-art and
providing up-to-date achievements in the distinguished fields.

4. Supercontinuum sources in mid-IR spectroscopy: an overview of state-of-

the-art applications
Supercontinuum laser sources have been used for applied IR spectroscopy (primarily near-IR)
for more than a decade. However, they are now at the stage of widespread adoption, becoming
standard laboratory equipment that can advance well-established spectroscopic techniques
and methods. In this section, we review the current state of supercontinuum-based mid-IR
spectroscopy and list the most valuable reports in categorised tables (see Tables 1, 2, and 3).
The topical tables contain a summary of the results and provide relevant information about the
application scenario and the source used; emission spectral ranges are indicated in brackets.

Table 1. Overview of mid-IR supercontinuum applications in direct absorption spectroscopy.

# Type of supercontinuum Application description Details Ref. Year
1 Step-index ZBLAN fiber Identification and Measurements performed Ke et al. [158]
based, custom, same as in differential damage in within C-H fatty acid and 2009
[54]; varying repetition vitro of lipids and proteins; cholesterol esters
rate in MHz and sub-MHz absorption spectroscopy absorption bands; results
range, 10.5 W average of the constituents of compared with thermal-
power (reduced to 1.5 W normal artery and and synchrotron-based
for the spectroscopic atherosclerotic plaque; systems; adequate
measurements); signal-to-noise ratio
(12500-2220 cm−1 ) achieved
2 Step-index ZBLAN fiber Qualitative and Identification and Cezard et al. [159]
based, custom; 10 kHz quantitative concentration estimation 2011
repetition rate, 490 mW supercontinuum laser of an unknown
average power; absorption spectroscopy multi-component
(5000-2860 cm−1 ) for a multi-component atmospheric gas-mixture
atmospheric gas mixture (demonstrated for
methane)
3 Step-index ZBLAN fiber Absorption measurements Noise and polarization Kilgus et al. [160]
based, commercial; of oils, polymers, aqueous characterized; application 2016
variable repetition rate solutions of acetic acid, in various scenarios
between 30 and 50 kHz, ethyl-2-cyanoacrylate in demonstrated; advantages
75 mW average power; transmission and and potential applications
(5900-2400 cm−1 ) reflection geometry defined
4 Step-index ZBLAN fiber Transmission Potentials of Ringsted et al.
based, commercial; 35 measurements of barley supercontinuum-based [161] 2016
kHz repetition rate, 60 endosperm and barley oil system for analysis of food
mW average power ; with further classification samples demonstrated;
(8335-2380 cm−1 ) technical issue of the
spectra distortion due to
the absence of pulse
demodulation put forward
5 Step-index ZBLAN fiber Gas detection and Cavity enhanced Amiot et al. [162]
based, custom; 100 kHz concentration spectroscopy for 2017
repetition rate, 160 mW measurements for multi-component gas
average power; acetylene and methane detection with sub-ppm
(11100-2700 cm−1 ) [see Fig. 10(a)] accuracy demonstrated
[see Fig. 10(b)]
6 Step-index ZBLAN fiber Multi-bounce ATR 3-times improved Gasser et al. [163]
based, commercial; 40 spectroscopy, detection limits compared 2018
kHz repetition rate, 75 quantification of hydrogen to thermal emitters
mW average power; peroxide aqueous demonstrated
(5715-2380 cm−1 ) solutions
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5238

# Type of supercontinuum Application description Details Ref. Year

7 Step-index ZBLAN fiber Multi-species gas sensing System for multi-species Jahromi et al.
based, commercial; based on supercontinuum gas detection of broadly [164] 2019
repetition rate 2.5 MHz, source and upconversion absorbing gas species
500 mW average power; detection (nitrous oxide, ethylene,
(6665-2380 cm−1 ) methane, ethane,
acetaldehyde)
demonstrated; high speed
( 20 ms) sensing of ethane
with 15 ppbv·s−1
sensitivity achieved
8 Step-index ZBLAN fiber Detection of multiple Importance of brightness Jahromi et al.
based, commercial; broadband absorbing gas highlighted; application [165] 2019
repetition rate 2.5 MHz, species with sensitivity in for quality control of
above 450 mW average the sub-ppmv level stored fruits demonstrated
power; (6665-2380 cm−1 ) including simultaneous
detection of ethylene,
ethanol, ethyl acetate,
acetaldehyde, methanol,
acetone, and water
9 Step-index ZBLAN fiber Sensitivity-enhanced 4-times enhanced Zorin et al. [166]
based, commercial; supercontinuum-based detectivity demonstrated 2020
repetition rate adjusted to FTIR instrument through the extension of
3 MHz, 475 mW average demonstrated, compared interaction path length,
power; (9090-2270 cm−1 ) to the conventional system exemplified for aqueous
formaldehyde series;
detection method based on
lock-in amplification
proposed and discussed
10 Step-index ZBLAN fiber Multi-species trace gas Importance of pulse Jahromi et al.
based, commercial; sensing based on a integration (using lock-in [167] 2020
repetition rate 2.5 MHz, high-repetition-rate demodulation)
500 mW average power; supercontinuum source demonstrated, detection
(6665-2380 cm−1 ) and a scanning grating limit in the order of 100
spectrometer (30 m ppbv Hz−1/2 for various
multipass absorption cell hydrocarbons, alcohols,
used) and aldehydes
demonstrated
11 Step-index tellurite fiber Gas sensing based on a Detection and analysis of Lemière et al.
based, custom; 80 MHz high-repetition-rate carbon dioxide and [168] 2021
repetition rate, 40 mW mid-IR supercontinuum methane and their binary
average power; laser source; feasibility of mixture using compact
(5000-2855 cm−1 ) multiple detection of multipass cell
greenhouse gases
demonstrated
12 Step-index ZBLAN fiber Multi-species trace gas Fast, sensitive and high Jahromi et al.
based, commercial; sensing (sub-ppmv Hz−1/2 resolution trace gas sensor [169] 2021
repetition rate 2.5 MHz, sensitivity) using a mid-IR for fruit quality
500 mW average power; supercontinuum source monitoring demonstrated;
(5000-2500 cm−1 ) and a Fourier transform balanced detection scheme
spectrometer employed; concentration
measurements (ethanol,
acetaldehyde, ethyl
acetate, ethylene, acetone,
methanol)
13 1. Step-index ZBLAN Fast-scanning Fourier Trace gas detection Abbas et al. [152]
fiber based, commercial; transform spectrometer (spectral resolution of 750 2021
repetition rate 2.5 MHz, based on MHz) using
450 mW average power; high-repetition-rate supercontinuum sources
(5000-2500 cm−1 ) 2. mid-IR supercontinuum beyond 5 µm wavelength;
Chalcogenide fiber based, sources for trace gas noise of various
custom (DTU Fotonik) detection (demonstrated laser-based spectroscopy
[80]; repetition rate 3 for ethyl acetate, ethane, methods compared;
MHz, 86 mW average nitrous oxide, sulfur supercontinuum as a
power; (6660-950 cm−1 ) dioxide) alternative for real-life
applications introduced
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5239

Figure
Figure 10
10 reproduces
reproduces recently
recently published
published and
and illustrative
illustrative results
results on
on high-resolution,
high-resolution, high-
high-
sensitivity
sensitivity (sub-ppm for acetylene and methane) cavity enhanced absorption spectroscopy
(sub-ppm for acetylene and methane) cavity enhanced absorption spectroscopy for
for
gas
gas measurements.
measurements. An An experimental
experimental system
system incorporating
incorporating aa monochromator
monochromator andand aa mid-IR
mid-IR
supercontinuum
supercontinuum laser
laser source
source is
is shown
shown in 10(a).
in10(a).

(a) Cavity-enhanced supercontinuum-based (b) Calibration curves for acetylene (top) and
absorption spectroscopy system methane (bottom) concentration series

Fig. 10.Broadband
10.
Fig. Broadbandsupercontinuum-based
supercontinuum-basedcavity
cavityenhanced
enhancedabsorption
absorptionspectroscopy
spectroscopyininthe
mid-IR spectralspectral
the mid-IR range [162], reproduced
range [162], with permission
reproduced from AIP
with permission fromPublishing.
AIP Publishing.

It has to be noted that in photoacoustic mid-IR spectroscopy till now only one remarkable
research
It has based on thethat
to be noted FTIR-photoacoustic
in photoacoustic approach has been reported
mid-IR spectroscopy till now[170]
only(Mikkonen et al.,
one remarkable
2018). The employed source was ZBLAN fiber based, same as in [162] (repetition(Mikkonen
research based on the FTIR-photoacoustic approach has been reported [170] rate adjusted
et
depending on the sample, from 70 kHz to 400 kHz); the emission range is from 12500 cm to
al., 2018). The employed source was ZBLAN fiber based, same as in [162] (repetition rate
−1

2703 cm−1depending
adjusted (measurements on thewere performed
sample, in two
from 70 kHzsub-bands, 5715-5000
to 400 kHz); cm−1 and
the emission 3175-2860
range is from
-1 to 2703 cm-1 (measurements were performed in two sub-bands, 5715-5000 cm-1 and
cm ). The research demonstrated cantilever-enhanced photoacoustic spectroscopy for broadband
12500
−1 cm
-1 ). The research demonstrated cantilever-enhanced photoacoustic spectroscopy for
gas sensing.cmAbsorption
3175-2860 measurements of water vapor and methane with significant signal
enhancements
broadband gas(by a factorAbsorption
sensing. of 70) compared to the conventional
measurements system
of water vapor andbased
methaneon a with
thermal emitter
significant
have been demonstrated.
signal enhancements (by a factor of 70) compared to the conventional system based on a thermal
emitter have been demonstrated.
Table 2. Overview of supercontinuum-based mid-IR hyperspectral imaging and microspectroscopy.
# Type Table 2. Overview ofApplication
of supercontinuum supercontinuum-based
description mid-IR
Details hyperspectral imaging
Ref.and
Year
microspectroscopy.
1 Step-index ZBLAN fiber Hyperspectral imager Importance of spectral Dupont et al.
based, custom; 40 MHz based on a bright brightness discussed; [171] 2012
# repetition
Type rate, spectral
of supercontinuum supercontinuum source
Application description microspectroscopy
Details Ref. Year
brightness of 300 and a monochromator demonstrated, exemplified
kW/(nm·M2 ·sr) at 2857 (PbSe detector used) Importance
for of spectral
hyperspectral imaging
cm−1Step-index ZBLAN fiber
given; (7145-2500 (transmission, mapping)
Hyperspectral imager ofbrightness discussed;
oil/water mixture; 2 nm
cm−1based,
) custom; 40 MHz
based on a bright spectral resolution, spatial
microspectroscopy
repetition rate, spectral
supercontinuum source resolution of around
demonstrated, 20
exemplified
Dupont et al.
1 brightness of 300 µmforverified
hyperspectral imaging
and a monochromator [171] 2012
kW/(nm·m2 ·sr) at of oil/water mixture; 2 nm
2 Step-index
2857 cm ZBLAN fiber
-1 given; Hyperspectral imaging
(PbSe detector used) Prototype of hyperspectral
spectral resolution, spatial Farries et al. [172]
based; repetition rate not using bright
(transmission, mapping) imager based on 2015
(7145-2500 cm-1 ) resolution of around
stated, 1.2 W average supercontinuum source, acousto-optic tunable filter
20 µm verified
power (0.9 mW at sample); exemplified for polymer and InSb camera
(5000-2220 cm−1 ) film imaging demonstrated (5 µm
(transmission, full-field) resolution stated)
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5240

# Type of supercontinuum Application description Details Ref. Year

3 Step-index ZBLAN fiber Hyperspectral microscopy Performances of QCLs, Lindsay et al.

based, custom; 30-350 based on acousto-optic thermal emitters, and [173] 2016
kHz repetition rate, >800 tunable filter and thermal synchrotron radiation for
mW average power (set to camera (transmission, microspectroscopy
30 kHz for imaging); full-field) discussed; imaging system
(5000-2220 cm−1 ) and its performances for
polystyrene samples
demonstrated (3.5 cm−1
resolution)
4 Step-index ZBLAN fiber Hyperspectral imaging Exemplified for colon Farries et al. [174]
based, custom; 30-300 system for rapid cells; high spatial 2017
kHz repetition rate, 1.1 W assessment of cells for resolution and high speed
average power (set to 30 cytological diagnosis imaging compared with
kHz and 50 mW for based on acousto-optic the FTIR system
imaging); (5000-2200 tunable filter and thermal demonstrated; potentials
cm−1 ) camera (transmission, for point of care screening
full-field) on live patient highlighted
5 Step-index ZBLAN fiber Broadband Prototype of low-NA Huot et al. [175]
based, commercial; upconversion-based (aberrated due to parabolic 2017
repetition rate 40 kHz, 100 imaging, mirror) hyperspectral
mW average power; proof-of-principle upconversion imager
(5550-2220 cm−1 ) (transmission, full-field) demonstrated; no spectral
diversification given, but
indirectly shown in images
(phase-matching
distribution)
6 Chalcogenide fiber based Multispectral tissue Proof-of-principle Petersen et al.
(tapered large-mode-area imaging of nontumoral demonstration of mid-IR [176] 2018
photonic crystal fiber from colon tissue section in the multispectral microscopic
highly purified diagnostically important imaging; compared to
Ge10 As22 Se68 glass), fingerprint region conventional FTIR system;
custom; 21 MHz (transmission, mapping) relatively low-noise
repetition rate, 25 mW images obtained, 12.4 µm
average power (see [116]); spatial resolution (at 1667
(5000-1335 cm−1 ) cm−1 ) stated
7 Step-index ZBLAN fiber Fourier transform infrared Chemical mapping of lipid Borondics et al.
based, custom; 4.15 MHz microspectroscopy vesicles in a liver [177] 2018
repetition rate of the pulse (transflection, mapping) demonstrated; compared
train, several satts of with synchrotron- and
average power (reduced by thermal-based
neutral density and instruments–improved
band-pass filters); signal-to-noise
(5000-2665 cm−1 ) ratio/shorter acquisition
times achieved; 3 µm
spatial resolution (at
around 2950 cm−1 ) stated
8 Step-index ZBLAN fiber Diffraction-limited Diffraction-limited Kilgus et al. [178]
based, commercial; chemical mapping microspectroscopy 2018
repetition rate 2.5 MHz, (reflection, spatial verified; imaging of red
500 mW average power; resolution of 2.8 µm at blood cells (spectrum of a
(6450-2220 cm−1 ) 2700 cm−1 ) based on single cell recorded, see
MEMS Fabry-Pérot filter details in Fig. 11) and
spectrometer various polymers
demonstrated; sensitivity
advantages over standard
equipment discussed
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5241

# Type of supercontinuum Application description Details Ref. Year

# Type of supercontinuum Application description Details Ref. Year
Active hyperspectral
9 Step-index ZBLAN
Step-index ZBLAN fiber
fiber Multimodal
Multimodal hyperspectral
hyperspectral Active
imagerhyperspectral
combined with Zorin et al. [179]
based, commercial; and structural imaging for imager combined with 2019
based, commercial; and structural imaging for 3D-tomographic modality
repetition rate 2.5 MHz, non-destructive testing in 3D-tomographic modality Zorin et al.
9 repetition rate 2.5 MHz, non-destructive testing in demonstrated;
490 mW average power; art diagnosis (reflection, demonstrated; [179] 2019
490 mW average
(9090-2275 cm−1 ) power; art diagnosis (reflection,
mapping) performancefor
performance forimaging
imaging
(9090-2275 cm-1 ) mapping) of art mock-ups
of art mock-ups (oil(oil
paintings)
paintings)reported
reported

10 Step-index ZBLAN fiber Combination

Combination ofof Aspects
Aspectsofofcombination
combination Zorin et al. [180]
based, commercial;
Step-index ZBLAN fiber hyperspectral
hyperspectralimaging
imaging discussed;
discussed;hyperspectral
hyperspectral 2020
repetition rate 2.5 MHz,
based, commercial; (reflection, mapping) and imager
imagercombined
combinedwith with
(reflection, mapping) and
490repetition
mW averagerate power;
2.5 MHz, optical coherence optical
opticalcoherence
coherence Zorin et al.
optical coherence
10 same
490asmW
in [179];
average power; tomography enabled by tomography
tomographydemonstrated;
demonstrated; [180] 2020
(9090-2275 tomography
brightnessenabled
of the by
same as incm −1 )
[179]; high correlative
correlativeimaging
imagingofof
(9090-2275 cm-1 ) source employed of the
high brightness polymers
polymersembedded
embeddedinin
source employed ceramics
ceramicsdemonstrated
demonstrated

40 0.10

35
0.08
30
Absorbance (a.u.)
Y coordinate µm

25
0.06
20

15
0.04
10

5 0.02

0
0 10 20 30 40 3200 3000 2800
X coordinate µm Wavenumber (cm−1)

(a) Global intensity mid-IR microscopic (b) Absorption spectrum of a single red
image of red blood cells on substrate, blood cell extracted from hyperspectral
obtained using mapping approach cube

PM
FPFS
CH
BS
ZBLAN
PM
SCL RO
PM
xy-stage

Fig. 11. Diffraction-limited supercontinuum-based

(c) Scheme of the optical reflection
setup: SCL - supercontinuum microspectroscopy,
Laser, PM - parabolic repro-
duced from [178]
mirror,with
BS -permission
beam splitter,from
RO -OSA.
reflective objective, CH - chopper, FPFS -
Fabry-Pérot tunable filter spectrometer.

Fig. 11. Diffraction-limited supercontinuum-based reflection microspectroscopy,

reproduced from [178] with permission from OSA.

Notably, most of the applications listed in Table 2 distinguish and emphasize the particular
importance of the high spectral brightness and beam quality (two sides of the same coin) of
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5242

Notably, most of the applications listed in Table 2 distinguish and emphasize the particular
importance of the high spectral brightness and beam quality (two sides of the same coin) of
modern supercontinuum laser sources for imaging applications. In the publication of Kilgus et
al. [178], mid-IR supercontinuum sources were demonstrated as a solution for eliminating the
trade-off—specific for standard FTIR spectral microscopes—between spatial (resolution) and
spectral (signal-to-noise ratio) performances. The practical aspects and signal-to-noise gains
enabled by this new source type are discussed. Figure 11 reproduces a layout of the all-mirror
(mirror optics was employed to avoid chromatism) hyperspectral mid-IR microscope based on a
supercontinuum source. The capabilities of the system were demonstrated by diffraction-limited
imaging of erythrocytes. A corresponding image is depicted in Fig. 11(a). Each pixel of the
system’s output contains a complete spectral information [see Fig. 11(b)] that is accessed by a
spectrometer (a Fabry-Pérot tunable filter spectrometer operating from 3.1 µm to 4.4 µm). The
reported spatial resolution of the system is around 4.5 µm.

Table 3. Overview of supercontinuum based mid-IR stand-off/remote spectroscopy.

# Type of supercontinuum Application description Details Ref. Year
1 Step-index ZBLAN fiber Stand-off diffuse reflection Stand-off system based on Kumar et al. [181]
based, custom; repetition spectroscopy of explosives monochromator (InSb 2012
rate 2 MHz (modulated at (TNT, RDX, PETN), detector, lock-in
500 Hz to reduce the fertilizers (ammonium demodulation) demonstrated;
thermal load), 3.9 W nitrate, urea) and paints measurements (high quality
average power; (automotive and military spectra obtained and verified)
(13330-2325 cm−1 ) grade) at the distance of 5 m
achieved, performances at
distances up to 150 m
predicted; importance of
spectral extension beyond 6
µm emphasized
2 Step-index ZBLAN fiber Sensitive stand-off Importance of filling the Kilgus et al. [182]
based, commercial; analysis of various spectral gap of QCLs 2018
repetition rate 2.5 MHz, samples (ammonium highlighted; robust design,
490 mW average power; nitrate, transparent acrylic verified stand-off spectroscopy
(8330-2175 cm−1 ) paint, black alkyd paint, and real-time capabilities [for
2-propanol) employing a monitoring the evapo- ration
low-cost MEMS of 2-propanol, see Fig. 12(b)]
Fabry-Pérot spectrometer at 5 m distances demonstrated;
[see Fig. 12(a)] noise characterized

The majority of the publications on the mid-IR supercontinuum generation imply potential
advances for stand-off detection and remote spectroscopic sensing. Nevertheless, up-to-date
only two reports (see Table 3) were presented [181,182]; both of them benefit from and
illuminate the practical significance of the directionality, brightness, and spectral coverage of
supercontinuum emission. Figure 12 illustrates the capabilities of supercontinuum-based remote
mid-IR spectroscopy exemplified for the latest publication (the optical scheme and time-resolved
stand-off measurements of 2-propanol evaporation are displayed).
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5243

ZBLAN 0.5 - 5 m
chopper
SC

FPFS

(a) Scheme of the supercontinuum-based stand-off

detection system, SC - supercontinuum, FPFS - MEMS
Fabry-Pérot spectrometer

(b) Time-resolved monitoring of the evaporation

process of 2-propanol at 5 m distance (18 sec
measurement)

Fig. 12. Supercontinuum-based

Fig.12. mid-IR stand-off
Supercontinuum-based mid-IR stand-offspectroscopy
spectroscopy[182],
[182],reproduced
reproduced with
with
permission
permission from SAGE
from Publishing.
SAGE Publishing.

In order to provide a full snapshot on the current state-of-the-art, it is worth to include

some near-IR
In order to realizations,
provide a full which are relevant
snapshot on the as important
current milestones in
state-of-the-art, theworth
it is development of
to include
IR supercontinuum sources. These works allow us to understand the state of supercontinuum-
some near-IR realizations, which are relevant as important milestones in the development of
based
IR IR spectroscopy
supercontinuum in general
sources. Theseand to extrapolate
works allow us to possible
understandperformance
the state ofofsupercontinuum-
similar mid-IR
implementations that have not been yet reported in this range but expected. We
based IR spectroscopy in general and to extrapolate possible performance summarise
of similar the
mid-IR
most remarkable reports in Table 4.
implementations that have not been yet reported in this range but expected. We summarise the
most remarkable reports in Table 4.

Table 4. Overview of featured near-IR spectroscopic applications of supercontinuum

Table 4. Overview of featured near-IR spectroscopic applications of supercontinuum sources.
sources.
# Type of supercontinuum Application description Details Ref. Year
1 # Soft-glass
Type ofphotonic-crystal
supercontinuum High resolution description
Application Performances of
Details Mandon et al.
Ref. Year
fiber based; custom, 142 Fourier-transform supercontinua for [183] 2008
MHz repetition rate, 25 absorption infrared Performances of
established techniques of
mW average power; spectroscopy (ammonia supercontinua
IR spectroscopyfor as
(14815-4545
Soft-glasscm )
−1 and acetylene
High overtone
resolution replacement of thermal of
established techniques
photonic-crystal fiber bands)
Fourier-transform sources demonstrated
IR spectroscopy as
based; custom, 142 MHz absorption infrared (high speed, high
replacement of thermal
Mandon et al.
1
repetition rate, 25 mW spectroscopy (ammonia sensitivity achieved);
sources demonstrated
[183] 2008
significant
(high speed,impacts
high of
average power; and acetylene overtone
possible extension
sensitivity towards
achieved);
(14815-4545 cm-1 ) bands)
mid-IR region
significant stressed
impacts of
2 Silica fiber based; 80 MHz Near-IR Fourier transform possible extension towards
High temporal stability of Michaels et al.
repetition rate, 6 W spectroscopy (methane mid-IR region stressed
supercontinuum sources [184] 2009
average power; and methyl salicylate) for time scales relevant to
(22220-4000 cm−1 ) using multipass FTIR demonstrated and
absorption gas cell (18 m); discussed; noise
in-deep noise characterised in
characterization provided comparison to the
tungsten lamp; drawbacks
and potentials for mid-IR
FTIR spectroscopy
distinguished
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5244

# Type of supercontinuum Application description Details Ref. Year

3 Standard single-mode Reflectance spectroscopy Beam quality Alexander et al.

silica fiber based (several of various samples (at 2 m characterised at 1.6 km [185] 2013
amplification stages), distance); for sensing, distance (Gaussian,
custom; up to 20 MHz beam delivered at distance symmetric, full angle
repetition rate, around 5 W of 1.6 km beam divergence 0.49
average power; mrad, M2 =1.26); active
(6660-4255 cm−1 ) spectral reflection
measurements of various
samples demonstrated and
verified; potentials as well
as limitations (i.e.
turbulence) discussed
4 Photonic-crystal fiber Supercontinuum laser Accuracy and feasibility Yoo et al. [186]
based, custom; up to 40 absorption spectroscopy of supercontinuum-based 2016
MHz repetition rate (10 of several simple diagnostic strategy studied
MHz default), 1 W hydrocarbon species and verified; applicability
average power; high (methane, acetylene, of the technique
stability and repeatability ethylene, propane) at demonstrated; potentials
stated; (10525-5880 various concentrations and for steady-state pyrolysis
cm−1 ) pressure conditions and gasification
applications highlighted
5 Thulium-doped fiber Transmission spectroscopy Prediction of mixed- Ringsted et al.
based, commercial; 35 of barley seeds using a linkage beta-glucan [187] 2017
kHz repetition rate, 120 supercontinuum laser content in whole barley
mW average power; seeds with high accuracy
(4760-3845 cm−1 ) demonstrated
6 Standard single-mode Spectroscopic Low-cost high pulse Dasa et al. [188]
silica fiber based, custom; photoacoustic imaging of energy supercontinuum 2018
30 kHz repetition rate, lipids in the first overtone developed and
pulse energy density 25 region using high pulse characterised;
nJ/nm (in 6060-5405 cm energy supercontinuum spectroscopic
−1 range); (6450-5265 (based on high pulse photoacoustic qualitative
cm−1 ) energy ns pumping) discrimination and
cross-sectional scanning
of lipids in the first
overtone transition band of
C-H bonds demonstrated
7 Standard single-mode Photoacoustic Suitability of super- Selvaraj et al.
silica fiber based, spectroscopy for online continuum-based sensing [189] 2019
commercial; 250 kHz multi-gas (carbon dioxide, for online monitoring for
repetition rate, >1.3 W methane, water vapor, operational large scale
average power; hydrogen sulfide) sensing biogas plants
(11110-3570 cm−1 ) with high-speed data demonstrated
acquisition, resolution,
and no interference from
humidity
8 Standard single-mode Short-range Gas absorption cross- Saleh et al. [190]
silica fiber based, custom; supercontinuum lidar (up sectional dependence on 2019
280 kHz repetition rate, to 10 m) for spectroscopic temperature exploited;
pumped by a 1 kW peak temperature advances over
power system; measurements in narrow-band lasers
(10000-6250 cm−1 ) combustion units at plant demonstrated;
environments (utilising simultaneous 3D mapping
absorption of water vapor) of temperature and
concentration for the
combustion diagnosis
proposed
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5245

#
Type of supercontinuum Application description Details Ref. Year
# Type of supercontinuum Application description Details Ref. Year
Standard non-zero
High pulse energy
dispersion-shifted Ex vivo (Adipose tissue)
supercontinuum
9 Standard non-zero
single-mode optical fiber vivoin(Adipose
Exand tissue)
vivo (Xenopus High pulse energy Dasa et al. [191]
developed for multi-
dispersion-shifted
based (several and in vivo
laevis (Xenopus
tadpoles, embryos) supercontinuum developed 2020
single-mode optical fiber laevis tadpoles, embryos) spectral
for multi-photoacoustic
spectral
amplification stages), photoacoustic microscopy Dasa et al.
9 based (several photoacoustic microscopy microscopy; high
photoacoustic quality
microscopy;
custom; 100 kHz of lipids in the extended [191] 2020
amplification stages),
repetition rate, pulse ofnear-infrared
lipids in the extended
using high high quality imaging
imaging over first over
custom;
energy100 kHz 18.3,
density near-infrared
pulse energyusing high first overtone
overtone transition
transition of of
repetition
1830 mW rate,average
pulse power pulse energy
supercontinuum C–H
C–Hvibration
vibrationbonds
bonds
energy density
µJ/nm; 18.3, 1830
(6945-5350 cm-1 ) supercontinuum demonstrated
demonstrated
mW average power µJ/nm;
(6945-5350
Standard cm −1 )
single-mode
System for multi-species
10 optical fiber based,
Standard single-mode Compact,
Compact, low-cost
low-cost System for multi-species Adamu et al. [192]
gas detection (ammonia,
custom;
optical fiber30-100
based, kHz all-fiber
all-fiber gas detection (ammonia, 2020
methane) reliable for
custom; 30-100
repetition kHz
rate, around supercontinuum-based
supercontinuum-basedgas gas methane)
continuousreliable for
monitoring
Adamu et al.
10 repetition
20 mWrate, around
average power 20 sensor
sensorforfor
detection ofof
detection continuous monitoringand [192] 2020
with high selectivity
mW average
(after power
gas cell (after
filled with multiple
multipleindustrial toxic
industrial toxic with high selectivity
sensitivity (4 ppm) and
gaspure
cell N
filled
2 ); with pure gasses
gasses sensitivity (4 ppm)
demonstrated;
N2 (6755-5880
); (6755-5880 cmcm-1 )−1
) demonstrated;

Analyzing
Analyzing thethe tables,
tables, we
we can
can note
note that
that the
the number
number of of publications
publications related
related to
to mid-IR
mid-IR spectroscopy
spectroscopy
is
is increasing annually, indicating a growing interest and development in this field.
increasing annually, indicating a growing interest and development in this field. Figure
Figure 13
13
complements
complements this analysis and shows the state of technology and academic impact as measured
this analysis and shows the state of technology and academic impact as measured
by
by the
the number
number of of publications
publications and
and citations.
citations. We
We believe
believe that
that the
the current
current progress
progress isis primarily
primarily
driven
driven by developments and commercialization of novel high-performance supercontinuum laser
by developments and commercialization of novel high-performance supercontinuum laser
sources,
sources, i.e.
i.e. their
their extending
extending availability.
availability.

50 25000

40 20000
Number of publications

Number of citations

30 15000

20 10000

10 5000

0 0
2002 2004 2006 2008 2010 2012 2014 2016 2018 2020 2002 2004 2006 2008 2010 2012 2014 2016 2018 2020
Year Year

(a) (b)

Fig. Current
13.13.
Fig. technology
Current state state
technology and academic impact:impact:
and academic (a) Number
(a) of scientific
Number of publications
scientific
by publications
year that contain keywords
by year "infrared
that contain supercontinuum",
keywords according to the "PubMed"
"infrared supercontinuum", according search
to
(primarily biomedical
the "PubMed" literature);
search (b) Citations
(primarily per year
biomedical (the number
literature); of times that
(b) Citations perayear
publication
(the
hasnumber
been cited by other
of times that publications)
a publication related
has beentocited
the search "mid-infrared
by other publications)supercontinuum",
related to the
according to "Dimensions"
search "mid-infrared research information
supercontinuum", database.
according to "Dimensions" research information
database.
Nevertheless, the absolute figures show that despite the growing number of reports on
supercontinuum generation (prevailing fraction of the scientific publications) and its advances in
theNevertheless, the absolute
mid-IR, the application figures
of this show that
technology despite
is still the growing
emerging number
at the step of beingofnoticed
reportsand
on
supercontinuum generation (prevailing fraction of the scientific publications) and
adopted by a broader community of spectroscopists. At the moment, the research is still very its advances
in the dominated
much mid-IR, thebyapplication of this
single groups, technology
which is stillthe
might explain emerging
unsteadyatdevelopment
the step of being noticed
of published
and adopted by a broader community of spectroscopists. At the moment, the research
papers (e.g. the drop in 2017). In addition, we can note that reported applications in the near-IR is still
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5246

and shortwave mid-IR still prevail over long-wavelength realizations. We attribute that to the
lag in commercialization of ultra-broadband sources, although, systems covering the entire
mid-IR fingerprint region were reported and successfully demonstrated. However, the situation is
expected to change as first commercial systems with the extended coverage appear [193,194].
Figure 13 was compiled using open data sources. The data on the number of publications
(primarily biomedicine related literature) were obtained from the PubMed database (the search
keywords are "infrared supercontinuum"); the data on the number of citations (for the keywords
"mid-infrared supercontinuum") were obtained using "Dimensions" research information database
[195].

5. Conclusions and outlook

This review has set a focus on various practical aspects and prospects of supercontinuum
technology that are relevant for mid-IR spectroscopy. Just as progress on the supercontinuum
generation in the 1970s was driven by the interests of Raman spectroscopy, we find that current
progress is accelerated primarily by interests of IR spectroscopy, although only a limited number
of groups had hands on this novel type of mid-IR laser source at the time of writing. In this
contribution, we aimed to introduce and demonstrate specific characteristics of supercontinuum
emitters to the broad spectroscopic community. For this purpose, we have analyzed, quantified
and illustrated typical emission properties of several commercial mid-IR supercontinuum sources.
Thus, spectral brightness, coverage, laser emission properties (in particular the M2 beam quality),
and stability (long- and short-term) have been investigated. In particular cases, we have provided a
comparison of the supercontinuum technology to standard, well-established and advanced mid-IR
spectroscopic equipment to highlight the emerging capabilities. In a detailed overview, we have
summarized and assessed the current state-of-the-art with a focus on highly promising reports and
achievements in the field of mid-IR spectroscopy. The review shows that the technology of mid-IR
supercontinuum generation offers novel, previously unavailable features and is sufficiently mature
to enter the applied field. The technology can compete in well-known application scenarios,
but it can also create new analytical methods. Thus, mid-IR supercontinuum laser sources are
candidates to at least fill the gap between quantum cascade lasers (QCL) and standard thermal
emitters or even potentially overcome the latter in particular cases. The main advantages are the
ultra-broadband spectral coverage, which also covers bands not available with QCL technology,
and superior brightness levels at a reasonable price per spectral band. In addition, the surveyed
work also shows the need for both further fundamental and applied research in this field. Further
extensions of the spectral bandwidth, commercialization of the sources covering the entire
fingerprint region, improvements of noise performance through tailoring the supercontinuum
generation dynamics are of particular importance. These steps will significantly stimulate the
application field.
Funding. Österreichische Forschungsförderungsgesellschaft (856896, 874787, 877481); State of Upper Austria
(Wi-2020-700476/3); Horizon 2020 Framework Programme (722380).
Acknowledgments. The authors thank Guillaume Huss from Leukos for the fruitful and detailed discussions and
providing the power spectral densities of various mid-IR supercontinuum sources used to calculate the spectral brightness
levels; Roozbeh Shokri and Reza Salem from Thorlabs for discussions and lending the InF3 fiber based supercontinuum
source; NKT Photonics and particularly Patrick Bowen for technical conversations and providing a low-cost mid-IR
ZBLAN based source; and Novae, in particular Marc Castaing, Nicolas Ducros and Kirill Zaytsev, for discussions
and providing the mid-IR supercontinuum generator (Novae Coverage) for our experiments and characterization. In
addition, Ivan Zorin acknowledges former SUPUVIR partners (an abbreviation for "SUPercontinuum broadband light
sources covering UV to IR applications") for establishing a firm scientific network in developments and applications of
supercontinuum sources; Ivan is grateful to be part of the community that generated many of the works reviewed in this
contribution. This work was co-financed by research subsidies granted by the government of Upper Austria.
Disclosures. The authors declare no conflicts of interest.
 Research Article Vol. 30, No. 4 / 14 Feb 2022 / Optics Express 5247

Data availability. Data underlying the results presented in this paper are not publicly available at this time but may
be obtained from the authors upon reasonable request.

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