Ref 1
Ref 1
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J. P. Marangos
Topical review
Electromagnetically induced transparency
J. P. MARANGOS
Laser Optics and Spectroscopy Group, Blackett Laboratory, Imperial
College, London SW7 2 B 2 , England
1. Introduction
Interference between alternative pathways in quantum-mechanical processes is
an ubiquitous effect in physics (for example [l]). This interference is analogous to
constructive and destructive interference between classical waves but, whilst with
classical wave interference it is the field amplitudes that are interfering in the
quantum case, however, we must invoke intuitively less definite quantities (e.g.
probability amplitudes) to explain quantum interference phenomena. Matter wave
interferometry, especially atom beam interference between spatially separated
beam paths, has recently received considerable theoretical and experimental
attention [2-41, not least because of the potential for the construction of ultra-
sensitive interferometers that might be used to measure atomic and molecular
interactions with extreme sensitivity [S] and to test fundamental aspects of
quantum mechanics (see, for example, the proposal in [6,7]). Another kind of
interference phenomenon, between transition pathways induced within the inter-
nal quantum states of atoms and molecules coupled to one or more laser fields, is
the subject of the present review. In particular, three-level atomic and molecular
systems coupled to two laser fields exhibit interference effects that can result in
cancellation of absorption at a resonance transition frequency and other modifica-
tions of the optical response.
It has been known for some time [8] that, if states of an atom are coupled via
several possible alternative transition processes, interference between the ampli-
tudes of these processes may lead to an enhancement (constructive interference) or
a complete cancellation (destructive interference) of the total transition probabil-
ity. These effects arise because in quantum mechanics it is probability amplitudes
12> T+F;k
channel (b)
)j continuum
hmuv\ Ihwuv
Figure 1. Interference between pathways in autoionization of an atom by ultraviolet
radiation. The ground state 11) is coupled to the continuum state IE2,k) via two
alternative pathways; channel (a) is direct photoionization by absorption of an
ultraviolet photon (WVUV), channel (b) is an indirect photoionization process in
which absorption of the ultraviolet photon (WVUV) results in excitation into bound
state 12) which is followed by a transition to the continuum state via the
interelectronic Coulomb interaction. The amplitudes due to these two channels
must be summed to give the overall photoionization amplitude; thus interference is
seen in the ionization rate.
(which may be positive or negative in sign), rather than probabilities, that must be
summed to obtain the total transition probability of a process.
An example of this in atomic systems is Fano [8, 91, interference seen for
radiative transitions to autoionizing states in atoms and also predicted in semi-
conductor quantum wells [lo], leading to asymmetric spectral profiles. Here
(figure 1 ) a doubly excited state of the atom 12) of energy E2, with a bound-state
character, lies in the continuum and is energetically degenerate with a continuum
state IE2,k) (at the same energy E2) to which it is coupled via the Coulomb
interaction between the two electrons. An ultraviolet electromagnetic field will
cause photoexcitation from the ground state 11) to the continuum state (E2,k ) . This
photoionization can proceed via two possible channels: firstly a direct photoioniza-
tion 11) + JE2,k ) or secondly an indirect process consisting of excitation 11) + 12)
followed by a rapid radiationless transition (caused by the interelectronic Coulomb
interaction) 12) + IE2, k ) . Interference occurs between these two channels with a
sign varying from constructive to destructive depending on the frequency of the
ultraviolet electromagnetic field.
This type of interference is deliberately induced by an applied laser field in
recent work concerned with the laser control of the optical properties of atomic
media. T h e cancellation of absorption for a probe field tuned in resonance to an
atomic transition, for which strong absorption would normally be expected, is
perhaps the most striking example. This process has been termed electromagneti-
cally induced transparency ( E I T ) [ l l , 121, the effect being caused by the inter-
ference between the coherences excited in the atom by the electromagnetic fields
and leading to an initially highly opaque medium being rendered almost trans-
parent. Similarly the refractive properties of the medium may be greatly modified
[13,14]; for instance the usual correlation of high refractive index with high
absorption can be broken, leading to the creation of media with very unusual
Electromagnetically induced transparency 47 3
Figure 2. The basic energy level schemes for three-level atoms interacting with two
near-resonance electromagnetic fields. In all cases, 11) is dipole coupled to 12), and
12) to 13), but 13) is not dipole coupled with 11) (metastable). The schemes are
defined by the relative energies of the three states: (a)a ladder or cascade system;
(b) a A scheme; (c) a V scheme.
the experimental techniques used rather than in any strict chronological order.
Thus first (section 3.1) some of the earlier experimental investigations of atomic
coherence effects are briefly reviewed. Then the first E I T experiments that
employed pulsed (section 3.2) and continuous-wave (CW) (section 3.3) lasers are
discussed. Related experimental work on amplification without inversion and
lasing without inversion is presented in section 3.4. Pulse propagation and
matched pulse effects are a development that connects E I T with recent work on
coherent adiabatic population transfer, and both theoretical and experimental work
will be discussed in section 3.5. Finally, in section 3.6, recent experiments that
have used E I T and related processes to enhance nonlinear optical processes (a very
promising area) will be presented.
T h e review is completed with a discussion and conclusion in section 4 that
overviews the work done so far and the prospects for further developments in the
near future.
2. Physics of EIT
2.1. The physical basis of electromagnetically induced transparency
There is a close link between E I T and other atomic coherence phenomena such
as coherent population trapping [32,35-371 and coherent adiabatic population
transfer processes [38-41]. I n all these processes, three-level atomic systems are
involved (or at least systems that can be adequately reduced to three levels when
interaction with the pertinent electromagnetic fields are considered). T h e usual
atomic dipole selection rules normally require that two pairs of levels are dipole
coupled whilst the transition between the third pair is dipole forbidden. In figure 2
we show the three basic level schemes for three-level atoms; all the level schemes
involved in the experiments discussed in this paper can be reduced to one or other
of these schemes. We label the levels Il), 12) and 13), where 11) - 12) and 12) - 13)
are dipole allowed but 11) - 13) is not since 13) is a metastable state. Classification
Electromagnetically induced transparency 475
of the schemes then depends upon the relative energies of these three states [31]:
(a) in a ladder (or cascade) scheme El < E2 < E3;
(b) in a A scheme El < E3 < E2 (although, in a symmetric A scheme, El and
E3 are almost degenerate);
(c) in a V scheme E2 < El and E3 (although again in a symmetric V scheme, El
and E3 are almost degenerate).
In a A or ladder scheme, 11) is normally the ground state of the atom and is
where the majority of the population (initially) resides. E I T is associated with A
and ladder schemes since in this process population transfer is not required (in
contrast with C P T ) and states 12) and 13) can remain (essentially) unpopulated
throughout the process.
T o understand more clearly how laser fields may interact with a three-level
atom and create coherent superpositions of the atomic basis states we shall first
consider C P T in a A scheme. A three-level A system (figure 3) consisting of states
[ I ) , 12) and 13) is coupled b y two near-resonance laser fields of strength (defined in
terms of the Rabi frequency [31]) Q1 (at frequency w l ) and Q2 (at frequency w2).
Defining the frequency of transitions between states as wl2 = (E2 - E l ) / h ,
~ 2 = 3 (E2 - E3)/h and ~ 1 = 3 (E3 - E l ) / h we can further define one- and two-
photon (Raman) frequency detunings as A12 = w12 - w1, 423 = w23 - w2 and
A = (wl2 - ~ 2 3 -) (w1 - w z ) . T h e Hamiltonian HO of the bare atom should be
modified to include the interactions due to the two couplings, that is
+ +
H = Ho Vl V2 (where the interaction V, = hQj). T h e eigenstates of this new
Hamiltonian will be linear superpositions of the bare atomic states [ I ) , 12) and 13).
For the situation of exact two-photon resonance that is A = 0 (or rather exact two-
photon resonance taking into account any light shifts) two of the eigenstates of the
+ +
total Hamiltonian HO Vl V2 turn out to be symmetric and antisymmetric
coherent superpositions of the two lower states of the bare atom basis that are of the
form:
+
where Q’ = (a: Qi)”2. Importantly no component of the bare atom state 12)
appears in these superpositions. These form eigenstates of the atom-field system of
which one (I+)) is coupled to the intermediate state 12) via the electric dipole
interaction whilst the other state (I-)) becomes decoupled (a so-called ‘dark’ or
‘trapped’ state). This can be seen if we form the dipole moment between I+) or I-)
with the remaining bare atom state 12) [31]. If the magnitudes of the coupling fields
Q I and Qr are appropriately balanced, the negative sign in the superposition of 11)
and (3) which form I-) will ensure that the corresponding dipole moment will
vanish. In effect the two terms that are summed to give the transition amplitude
between 12) and I-) are of equal and opposite magnitude, and hence the total
amplitude will vanish. State I-) is often referred to as a non-coupled state (INC))
whilst I+) remains coupled to the electromagnetic fields (IC)).
In the above description the situation has been simplified by ignoring the fast
time development (at frequencies E l / h and E3/h) of the states in the superposition
in equation (1) (these terms will in fact disappear when the dipole moments are
476 J . P. Marangos
I 3)
Figure 3. The basic A (Raman) scheme leading to coherent population trapping. The
applied fields need not be in single-photon resonance, but the two-photon (Raman)
resonance condition should be met in this three-level system. In a CPT experiment
the laser fields Ql and Q2 are of comparable strength that this is sufficient to saturate
the two-photon transition.
formed). On the assumption that a steady-state situation has been reached, the
superposition state INC) will acquire all the population of the system through the
action of optical pumping (spontaneous emission from 12) will populate INC) but
there is no absorption process from J N C ) to 12) to depopulate it).
In the usual C P T scheme, 521 % 522, that is both coupling strengths are of
comparable magnitude, whilst the fields are also strong enough to reach the two-
photon transition saturation condition. In fact this does not necessarily require
that the fields are sufficient to saturate the single-photon transitions 11) - 12) and
12) - 13) since, under the two-photon resonance condition, state 12) can be
adiabatically eliminated and so does not enter into the consideration of the
coupling between atoms and fields.
In the C P T system, interference effects arise from both the coupling fields
since they are of comparable strength. If only one of the fields, that is 522, is strong
such that 521 << 522, then only interference effects due to processes driven by 522
will be important. This is the situation in E I T schemes and this close connection
between E I T and C P T has been discussed by a number of workers (for example
[32,42]). Typically in a C P T scheme the states 11) and 13) are Zeeman or hyperfine
sublevels of the ground state and are thus both initially populated. I n contrast, in
many E I T schemes, 13) is an excited state and has no population at any time during
the process. Unlike the case of C P T , where the time scale for population trapping
in the INC) state is several radiative lifetimes, in the case of E I T the effect is
established (within a single atom) in a time on the order of l / & which is generally
much faster. Comparison with coherent adiabatic population transfer schemes
(e.g. stimulated Raman adiabatic passage (STIRAP)) [38,39] also shows that the
E I T situation is equivalent to the initial stages in the population transfer process
when the counter-intuitively sequenced laser pulses satisfy the condition 521 << 522.
T h e interference associated with E I T arises because the transition amplitude
between 11) and 12) includes, as well as a term due to the resonant field 521, an
additional amplitude due to the presence of the other field 522. This additional term
has a negative sign with respect to the first and hence in an ideal situation will
Electromagnetically induced transparency 47 7
13d>
12d>
Figure 4. (a)The basic scheme for an EIT experiment, illustrated here in a A system in
the bare states. The field coupling 11) to 12) is a relatively weak probe Qp (equivalent
to Q,), whilst the field coupling states 12) and 13) called the coupling field QC
(equivalent to 0 2 ) is strong. This makes the adoption of the dressed-state basis
logical as illustrated in (6). (b) The dressed states labelled here as (3d) and 12d)
(referred to as) . 1 and Ib) in the text); destructive interference between the probe
absorption amplitudes due to these two dressed states leads to EIT.
cancel the first term completely. In the case of EIT, since the field Q2 is large (in
EIT experiments, 0 22 is usually called the coupling field and labelled Qc, and Q1 is
a weaker probe field labelled Qp), it is logical to choose the dressed state basis [21]
to analyse this system (figure 4); on this basis, upper states form a coherent
superposition, which for a resonant coupling 4 2 3 = 0 is of the form
or alternatively we can define the bare atomic states in terms of INC) and IC).
Thus, for example, state 11) (atom ground state) can be written
478 J . P . Marangos
For the case << Q2 it is clear from equation (4) that 11) will be almost equivalent
to INC) and thus (for two-photon resonance and a metastable state 13)) absorption
vanishes.
Alternatively, if the E I T process is viewed within the atomic bare-state basis
(rather than the dressed states), the so-called ‘coherences’ can be seen as being the
quantities pertinent to the interference. These coherences can be thought of, in a
semiclassical picture, as associated with the oscillating electric dipoles driven by
the coupling fields applied between pairs of quantum states of the system, for
example );1 - I j ) . Strong excitation of these dipoles occurs whenever electromag-
netic fields are applied close to resonance with an electric dipole transition between
two states. If there are several ways to excite the oscillating dipole associated with
Ii) - l j ) , then it is possible for interference to arise between the various contribu-
tions to this dipole, and these must be summed to give the total electric dipole
oscillation between );1 and l j ) (see figure 7 later). This is directly analogous to the
Fano [8] effect in autoionization, to the classical interference proposed in ideal
plasmas [15] and to effects discussed in the context of laser-induced continuum
structure [34].
Of course, formally coherences are identified with the off-diagonal density
matrix elements p~ formed by taking bilinear combinations of probability ampli-
tudes of two quantum states of the system (i.e. the weighting factors associated
with the outer products such as l i ) ( j l ) [45]. Off-diagonal elements of the density
matrix play a critical role in the evolution of an atom coupled to electromagnetic
fields [46]. Many calculations of atomic coherence effects and of E I T (as well as
general nonlinear optics and laser action) in three-level systems are therefore
developed in terms of the density matrix [14,47-49]. This approach also naturally
lends itself to the inclusion of dampings that cause the decay of populations and
coherences (e.g. radiative decay and collisions) [46]. Although convenient it is by
no means essential to use a density matrix approach and many theoretical
treatments that give clear physical insight, have been performed in terms of
probability amplitudes (for example [12,20,21]). Additional physical insight has
also been obtained by adopting other alternative approaches, for instance by a
careful consideration of the Feynman diagrams representing the various processes
involved that lead to interference [42,44], or by applying a quantum jump
approach [SO]. In all cases the predictions are essentially identical.
T h e magnitudes of the relevant density matrix elements can be computed from
the basic coupled evolution equations (the Liouville equation) [31,45] and are
found to depend upon parameters that are controllable within an experiment (e.g.
detunings and laser intensities). In figure 5 we show a prototypical E I T scheme (in
this case a ladder configuration, but entirely equivalent to the A schemes discussed
so far if 12) is higher in energy than the metastable state 13)). T h e detunings
between the fields E l at w 1 and E 2 at w 2 with respect to the associated transition
frequencies w l 2 and ~ 2 are 3 defined by 4 1 2 = w 1 2 - wl and A 2 3 = ~ 2 =
3 w 2 as above.
T h e Rabi frequencies are Q l and s 2 2 respectively. I n addition to dependence on
these laser properties the E I T will also depend critically on atomic parameters. For
instance since perfect absorption cancellation depends on the metastability of (3)
any radiative or collisional decay of this state will lead to finite absorption even at
Electromagnetically induced transparency 479
Figure 5. Illustration of a prototypical scheme for EIT, in this case a ladder (cascade)
system is shown. T h e single-photon detunings dl2 and 4 2 3 (defined in text) are shown.
zero detuning Awl = Aw2 = 0 . E I T will manifest itself in the value of the density
matrix element p12 whose real and imaginary parts should both vanish at zero
detuning (i.e. the coherence is cancelled by the interference of the pathways that
can excite it). A set of coupled equations connecting the density matrix elements,
for example p l 2 , p23 and ~ 1 3 and
, their temporal derivatives can be written down
and solved for various sets of conditions by either analytical or numerical means. It
should be noted that the interference that leads to E I T arises from the existence of
coherences p23 and pi3 that are coupled to p l 2 . T h e coherence pi3 between the
ground state 11) and metastable state 13) is present only because of the additional
laser coupling. T h e contribution to the coherence p i 2 from the coherences p23 and
p13 cancels with the direct contribution driving this coherence due to the applied
probe field (at frequency wl).
If a steady-state limit is assumed, all the derivatives in the density matrix
elements vanish; in this case the solution of coupled density matrix equations is
greatly simplified. This can be solved exactly usually under the additional
assumption that only the coupling field SZC is strong and hence is the only field
that must be retained to all orders. This solution is frequently obtained by using an
algebraic manipulation programme to invert the super-matrix resulting from the
set of equations [Sl]. These solutions yield the steady-state populations and
coherences (on- and off-diagonal density matrices respectively) and in particular
give the appropriate value of p12 (the coherence associated with the transition at the
probe frequency) that is of direct interest in describing E I T . T h e expression that i s
derived for p l 2 will include a number of terms in the various parameters (e.g. Qc:
and A ) that will lead to cancellation of its value (both real and imaginary parts)
when in two-photon resonance.
A time-dependent calculation is of course appropriate if there are time-
dependent laser pulses coupling with the atom. This is vital for modelling the
results of pulsed laser experiments and to account for transient effects correctly.
Some time-dependent calculations have been made but, unless restrictive simpli-
fying assumptions are applied [52], these calculations must be performed numeri-
cally rather than analytically. In most cases the results of the time-dependent
480 J. P . Marangos
(5)
where p12 is the electric dipole moment of the probe transition, A , j are the
detunings defined in section 2.1, and r2 and r3 are the radiative decays of states
12) and 13) respectively. In [12] these were derived using the equations describing
the time-dependent atomic bare-state amplitudes in a steady-state situation with
monochromatic coupling fields and with no collisional or Doppler broadening
included. Of course, identical expressions are obtained using a density matrix
approach. These susceptibilities are plotted in figure 6 as a function of detuning
Electromagnetically induced transparency 48 1
4 r
-20 -1 0 0 10 20
12
Figure 6. T h e dressed susceptibilities are shbwn for a three-level ladder with the
coupling laser in exact resonance (423)and with the probe laser tuned over the
ranges shown (in units of the decay rate 712 between states 12) and 11)). T h e
coupling field Rabi frequency Szc = 1Oy12 in these plots. (a) T h e imaginary part
(Im x!;)) of the dressed linear susceptibility that determines the absorption in the
medium; note the vanishing value at exact resonance due to destructive interference.
( b ) Rex:)) that determines the dispersion in the medium. (c) T h e third-order
dressed susceptibility Ixg'I that characterizes the coupling strength in the four-wave
mixing process; note the enhancement of this quantity at exact resonance due t o
constructive interference.
412 with A23 = 0 (coupling field resonant). This is a striking result when compared
with the case when no coupling field is present (a2= 0) [12]; the absorption
vanishes at exact resonance (if 13) is perfectly metastable). Simultaneously the
dispersion is modified so that, although still zero at line centre as in the uncoupled
case, the group velocity (dependent upon the slope of R e x ( ' ) ) can become
anomalously low [62] where absorption has vanished.
T h e consequence of this transparency is that a medium that would otherwise be
optically thick is now rendered transparent (or at least the opacity is greatly
reduced). T h e reduction in absorption is not merely that caused by the effective
detuning induced by the Autler-Townes splitting of the dressed-state absorption
peaks, that is the absorption that would be measured if the probe field were
interrogating the absorption coefficient of the medium in the wing of the absorp-
482 J . P. Marangos
Figure 7. (a), (b) T h e first two diagrams for a perturbative expansion of terms
associated with the linear susceptibility in the dressed system; there are an infinite
number of higher order terms of the same type as, ( 6 ) involving the exchange of an
even number of photons from the coupling field with the atom. (c), (d) T h e first two
terms associated with a perturbative expansion of the nonlinear susceptibility in the
four-wave mixing process. Note that in this case there will be an infinite number of
terms (like (d)) associated with the exchange of an odd number of photons from the
coupling field with the atom.
the 11) - 13) transition (this will be referred to as the two-photon coupling). In
addition to the dressed linear susceptibility, given by equations (S), which
describes the response of the medium to a weak probe at w1, there is now also a
dressed nonlinear susceptibility that describes the coupling of the atom to the four-
+ +
wave mixing process w1 = w, wb w2. This can be computed [12] along similar
lines to the nonlinear susceptibility and yields the result
(6)
where the sum on the right-hand side represents the contribution to the nonlinear
~
susceptibility of all the states of the atom; the fields at frequencies w, and wb are
close to two-photon resonant with 11) - 13) and are necessary to complete a four-
wave-mixing scheme with w2 in order to generate a field at frequency w1. This
nonlinear susceptibility is plotted in figure 6 (c); although similar to Im xD
(1) (figure
6 ( a ) )in the sense that the response displays the familiar Autler-Townes splitting,
484 J . P . Marangos
characterizes the reabsorption and wave-vector mismatch in the medium, and xD (3)
the coupling strength that generates the new field. Thus we can see the importance
of the destructive interference in the value of xg’ over the frequency range where
xg) experiences constructive interference. This enhances the generation efficiency
(in principle) in a Doppler broadened medium (see below) by many orders of
magnitude compared with the case with no coupling field causing a dressing of the
medium. Within the enhancement in &) are both the effect of reduced absorption
and the imposition of essentially perfect phase matching for all the resonant fields
(residual mismatch arising only through the dispersion caused by the remaining
off-resonance states). These effects were first suggested as a means to enhance
nonlinear optical frequency conversion efficiencies b y Tewari and Agarwal [75]
and by Harris et al. [12] and have been further discussed by several workers
[ S l , 76-79].
Propagation of two coupled pulses in a A (Raman) type of system has recently
been discussed by Harris et al. [53,54] and Eberly et al. [SS]. This Raman scheme
is equivalent to E I T in the limit where one of the fields is a weak probe and the
other a strong-coupling field. However, if both fields 521 and 522 are strong, the
dressed atomic system reacts back on the field modes in such a way as to result in
lossless propagation through the medium for both the fields. A proper insight into
this process is best obtained by thinking in terms of C P T . Essentially the coupling
laser fields cause the formation in the atomic system of coupled IC) and uncoupled
INC) coherent superpositions of the bare atom lower states. However, there is
additionally a strong coupling between these atomic states and the two driving
fields. Hence there are also formed stable normal modes of the driving fields, one
of which is uncoupled from the ‘uncoupled’ atomic state and the other of which is
‘uncoupled’ from the coupled atomic state. These new field modes result in the
lossless propagation of pulses through a normally ‘lossy’ medium once a certain
preparation energy has been extracted from the laser fields [.56]. Other work on
matched pulse propagation in a double-V system has also been reported recently [80].
(for example [23,31,81]), radiative decays of state 13) (e.g. on the 13) - 11)
channel), the existence of additional photoionization channels [82], collisions
[12,58] and phase diffusion of the laser field causing deviation from the transform
limit. Therefore in experiments these parameters need to be controlled by
choosing appropriate atomic systems, density ranges, laser intensities and laser
system parameters. In general experiments with C W lasers, in which phase
fluctuations can be made small with laser bandwidths reduced to the 1 M H z
level or less, most fully approach the steady-state monochromatic limit explored in
the elementary steady-state theory of these processes.
In many experiments, (inhomogeneous) Doppler broadening presents a serious
limit since it introduces a randomization in the effective laser detunings over the
ensemble of atoms in the sample [12,83,84]. Various methods have been employed
to eliminate this effect, that is working in Doppler-free configurations [85,86], or
using cooled atoms trapped in a magneto-optical trap [87,88]. Alternatively by
working with a coupling Rabi frequency larger than the width of the (Gaussian)
Doppler profile the influence of inhomogeneous broadening can be, in effect,
overcome [12]. T o generate Rabi couplings of greater than the Doppler width
(0.03 cm-') a C W laser, with a power typically of 1 W or less, must be focused
fairly tightly. This may lead to undesirable effects such as defocusing due to the
interplay between the dressed refractive index and the transverse intensity varia-
tion across the beam waist in the region of the focus [86]. For pulsed lasers, with
intrinsically high peak power, it is not generally necessary to focus the laser to
achieve the required intensity and thus the defocusing effects are not important
and there is also the important advantage that large numbers of atoms will be
within the dressed ensemble.
Pulsed laser E I T effects are not best modelled by a steady-state treatment.
Although pulsed laser bandwidths are inevitably larger than those of CW lasers
provided that the laser is transform limited the E I T effect is not reduced. Some
recent calculations [51,78] have been somewhat artificial in including relatively
large laser linewidths pertinent to the pulsed laser in a steady-state calculation. In
fact, provided that the laser is single mode and therefore transform limited (i.e.
without excess phase fluctuation), the dephasing introduced by the laser band-
width will not sufficiently disturb the phases of the coherences responsible for
interference within the interaction time scale (i.e. the duration r p of the pulse). I t
should also be appreciated that hyperfine sublevels will in general cause dephasing
of coherences on a time scale given by the inverse of their frequency separation
Awhf [31]. In a pulsed excitation the dephasing due to hyperfine levels within the
laser bandwidth will therefore be negligible provided that the interaction time
7p < l/Awhf (i.e. if the hyperfine splittings are sufficiently small).
In practice, incorporation of laser linewidths is most usually made via the
Wiener-Levy phase diffusion model (for example [51,78,89-911). In this way
the laser phase diffusion can be added directly to the relevant density matrix
coupled equations. This model, however, predicts Lorentzian laser linewidths, and
this may severely overestimate the line wing of the laser [91]. This leads to overly
pessimistic predictions about the effects of laser linewidth in the large G?c limit
where most pulsed laser E I T experiments need to be performed in order to
overcome the Doppler restrictions. More realistic phase diffusion models are
available [92-941 but are in general harder to implement in a calculation.
486 J . P. Marangos
3. Experimental work
3.1. Related atomic coherence experiments
T h e first experimental work on laser-induced atomic coherence dates back to
the 1970s. Evidence for atomic coherence induced by the illumination of atoms by
a modulated optical lamp in conjunction with resonant radio-frequency fields
was reported still earlier [95]. Other relevant early work includes the investigation
of dressing of two-level systems by strong microwave fields (Autler-
Townes splitting) [96], and work on photon echoes in two-level systems [97].
Mollow [98,99] reported novel features, subsequently termed the Mollow triplet,
of resonance fluorescence in a two-level system. Much work on two-level systems
has been carried out since (see for instance the review and books given in
[31,100,101] but, although two-level systems remain a subject of considerable
interest (e.g. in dressed-state lasers and quantum optics experiments), our concern
here is primarily with three-level systems (and in some cases with four-level
systems).
Atomic coherence and interference in three-level systems was first seen
experimentally in the work of Orriols and co-workers [35,102,103] in Pisa and
Gray et al. [lo41 in Rochester. T h e Pisa group performed experiments that
established coherence between the Zeeman split lower levels of a sodium atom
using a multimode laser. By employing a spatially varying magnetic field they were
able to observe a series of spatially separated dark lines (resonances), correspond-
ing to the locations where the Zeeman splitting matched the frequency difference
between modes of the coupling laser. This situation corresponds to a two-photon
resonant (Raman-resonant) A scheme and thus this is the first experimental
observation of CPT. T h e experiments of Gray et al. [lo41 are similar to this but
involved establishing coherence between the hyperfine lower levels of Na.
In essence in these experiments the laser fields couple to the atoms to create
superpositions of the two ground states. One of these superpositions can interact
with the fields (see section 2.1), a so-called ‘bright’ state (i.e. the coupled state IC)),
but the other does not because of cancellation of the two driven dipoles and is thus
termed a ‘dark’ state (i.e. the non-coupled state INC)). Once formed, the popula-
tion in the system will all be optically pumped into this dark state, in a matter of a
few times the radiative decay rate. Once in the dark state there is, by definition, no
process to remove the population and so there is a ‘trapping’ of the population in
this state. There has been a considerable body of experimental work carried out on
C P T and its applications (see [32] for a full review).
Recently the basic idea of C P T has been utilized in systems with time-varying
optical fields to yield very efficient excitation of atomic and molecular states
[38,40,41]. In these coherent adiabatic population transfer schemes (e.g.
STIRAP) the non-coupled ground-state superposition I NC) of C P T is evolved
in time from being a pure state of the lowest state 11) to being a pure state of the
upper state 13) as the relative strengths of the (strong) laser couplings vary. This is
achieved by employing counter-intuitive pulse sequences, typically with identical
Gaussian pulses, in which the coupling s22 reaches its peak value around the time
that 521 is just switching on and has decreased back to almost zero when the latter is
still just passing its peak. In his way the dark state INC) in equation (3) is initially
almost purely bare state 11) (the initial state of the system), then evolves through
being an admixture of 11) and 13) whilst both fields are strong and finally
corresponds to being purely state 13). T h e bright state IC) remains unpopulated
Electromagnetically induced transparency 487
throughout the process. Recently work has been performed which demonstrates
the utility of these effects in laser cooling of trapped atoms in a technique called
velocity-selective coherent population trapping (VSCPT) [l OS-1071.
degree of transparency induced when the coupling laser was applied at a high
power in this scheme was very high (a factor of much greater than exp (10)).
These two experiments serve to demonstrate the principle of E I T in a three-
level system. They also indicate how E I T can occur for both autoionizing and
collisional broadening of level 12). Importantly, in these experiments, pulsed lasers
were employed; although in both cases the coupling laser was nearly transform
limited, the probe laser needed no special characteristics to demonstrate the effect
(other than that its bandwidth was less than the width of the transparency hole).
Experiments using pulsed lasers continue to be important, most especially in the
context of nonlinear optics (section 3.5) and matched pulse propagation (section
3.6). A related resonant E I T scheme in Pb has more recently been explored by
Kasapi [110] as a technique for enhanced isotope discrimination. This method
utilized the resonant opacity of a low-abundance isotope (207Pb)at the frequency
where the commonest isotope in their sample (208Pb)is transparent.
state 12) of the system [114]. In this experiment an enhanced index of refraction
was found at frequencies where the absorption was zero.
Results of experiments on the R b A scheme also prove to be consistent with
theory with transparency being observed at the probe line centre with a width and
depth in reasonable agreement with the steady-state calculation [l 111. In the case
of the A scheme, co-propagating beams leads to a Doppler-free situation, possible
again because of the near equality of the probe and coupling laser wavelengths. As
mentioned before, because of the elimination of Doppler effects, it was possible to
employ very-low-power coupling lasers for these experiments. This was exploited
by the same workers to perform an experiment that stresses the quantum
interference nature of the E I T effect. By employing a coupling laser strength
SZc < 7 1 2 (i.e. the Rabi splitting is too small to give rise on its own to any significant
absorption reduction) a well developed transparency, with a depth limited only
by the laser linewidths, was reported [112]. This experiment illustrates clearly how
the additional coherence due to the coupling laser causes interference that cancels
the effect of probe absorption.
Recently work has been reported on E I T (and C P T ) in Rb and C s A schemes
for cold atoms confined in a magneto-optical trap ( M O T ) [87,88]. In the R b
system a Zeeman scheme has also been studied [115]. T h e novelty here is that the
trapped atoms are very cool (i.e. Doppler broadening is almost absent) and the
system is collisionless, making it close to ideal. Work has been carried out that
exploits these features to study the nonlinear absorption and dispersion of cold R b
atoms [116]. In cold Cs atoms in a M O T the nonlinear sum rule [117] for E I T -
type situations has been experimentally verified [118].
subsequent work this issue was addressed and firmer evidence for inversionless
conditions were established by accompanying measurements of absorption [121].
A similar scheme in K vapour has been investigated more recently by Kleinfeld
and Streater [122]. Amplification of the probe laser is again seen but, although
these workers do not experimentally confirm the absence of inversion, they
support their claim that this is indeed amplification without inversion by perform-
ing careful numerical analysis of the system with results that are comparable with
the experiment.
Clear-cut evidence for amplification without inversion has been found in other
systems. Working with a A scheme in Na, with additional incoherent pumping into
the upper state, Fry et al. [123] have seen atomic coherence effects leading to
amplification without inversion. That the atomic coherence effect is responsible
was confirmed by switching the coupling field on or off and observing that
amplification is only possible when the field is present; when this field is absent
the large population always present in the lowest state leads to absorption of the
probe. Other schemes showing unambiguous amplification without inversion have
also been reported. Picosecond pulses were used to excite atomic coherence among
the Zeeman sublevels of the Na ground state and amplification without inversion
was seen and carefully confirmed Nottelmann et al. [124]. Amplification without
inversion has also been demonstrated in a transient scheme in '12Cd through the
formation of a linear superposition of coherently populated Zeeman sublevels by
van de Veer et al. [125]. In this case, nanosecond dye lasers were used and the
coherent nature of the process was proven by the dependence of the gain on
the delay between coherence preparation and probe pulse and the magnitude of the
Zeeman splitting which controls the period for coherent transfer of population in
the atom. Recently a double-A scheme in He, driven by 877.9nm radiation in a
He-Ne discharge, was used to observe amplification at both 1079.8 nm and 61 1 nm
(up-conversion); here the evidence for amplification without inversion rests on
comparison with calculation [126].
The next step beyond amplification without inversion is to demonstrate lasing
without inversion by incorporating the gain medium within an optical cavity. In
the two experiments [23,24] where this has so far been demonstrated, amplifica-
tion without inversion was first proved using a probe through the medium, and
then the cavity was formed and lasing observed even under conditions where no
inversion is possible. T h e first of these experiments was in a V scheme formed on
the D1 and D2 lines of 87Rb,with incoherent pumping from the F = 2 hyperfine
level into the upper state of the D1 transition (lasing transition). Laser diodes were
used for all the coherent and incoherent fields. T h e incoherent pump was
generated by injecting white noise into an acousto-optical modulator modulating
one of the diodes. This work was therefore also the first experiment to achieve
amplification without inversion using diode lasers. An important conceptual
advantage of the V scheme is that there is no dressed basis within which a hidden
inversion might reside; thus there is in principle true inversionless gain. This
scheme can be considered in simplified form as a four-level system (three levels
coherently coupled and a fourth coupled via the incoherent field). There are,
however, 32 hyperfine sublevels that must be considered in a detailed analysis of
this system, which was carried out by Zibrov et al. [23] to yield predictions in good
agreement with their experiment. Subsequently work was reported by
Electromagnetically induced transparency 49 1
also shown that the delay time is connected to the attenuation of the transmitted
pulse and the Lorentzian linewidth of the forbidden 11) - 13) transition via the
relation In (EOut/Ei,,)= -713Tdelay. This has subsequently been developed to sug-
gest a general method for measuring Lorentzian linewidths [129].
Harris [69] has examined theoretically the prospects to control refractive index
using strong off-resonance pulses. In this calculation it is shown that the off-
resonance bound and continuum states lead to Stark shifts of the 13) and 11) states
that can be compensated by detuning the lasers from exact (low-field) Raman
resonance. If this is done, the additional coherence pi3 will lead to EIT-like
modification of the refractive index experienced by both pulses. This extends to
the situation for which the probe pulse is also strong. With both pulses strong,
Harris predicts that off-resonance C P T is feasible. Formation of an off-resonance
population trapped state is an important aspect of the experiment investigating the
elimination of optical-self focusing [1281 in which nonlinear refractive index effects
would lead to self-focusing, filamentation and beam break-up of the strong probe
field were it not for the formation of the coherent population trapped state.
photon resonance with ls-2s), generating a field at 103nm. Both the laser fields
used in the frequency mixing were derived from single-mode pulsed dye lasers. An
atomic H beam was specially constructed to increase the beam density and path
length so that these effects could be studied from the optically thin to the optically
thick limits [82]. T h e coexistence of undissociated H2 molecules in these systems
causes some additional effects that have also been studied in [133]. Photoionization
by the 243nm field was studied in the same experiments and shows an Autler-
Townes doublet structure. Both the sum-frequency mixing and photoionization
results agree qualitatively with the predictions of a steady-state calculation, but
this agreement is improved further if a time-dependent calculation is made [134].
In this scheme, photoionization of the 3p state was an order of magnitude greater
than that from the 2s state; this is important since the 1s-2s coherence must be
preserved for the E I T effect to survive and so decay due to photoionization is
critical. However, so long as this decay rate is significantly less than that affecting
the 3p state, the destructive interference in the absorption will persist and still lead
to enhancement of the frequency mixing.
Evidence for a quantum interference effect in the photoionization channel
arising from competition between the excitation of 2s atoms by either two photons
at 243 nm or a photon at 655 nm and another at 121.6 nm (the generated field) has
also been found [135]. This manifests itself when the product of N L (atom
density x path length) is increased from 10" to 10'' cm-I. At low values of N L
(optically thin) the Autler-Townes structure is seen in the photoionization
frequency response but, as N L is increased such that greater intensities of vacuum
ultraviolet radiation are generated, the channel for ionization at the position of the
Autler-Townes satellites cancels that driven by the laser field, and these features
disappear. Similar quantum interference effects affecting the generated field are
found to lead to a limiting density for resonantly enhanced four-wave mixing in a
scheme in R b [136]. This latter work, however, did not employ a single-mode
coupling laser and the low limiting R b concentrations (less than lo1' cmP3) found
may not be reflected in situations where E I T is present.
Electromagnetically induced phase matching was observed in an off-resonance
four-wave mixing scheme in 208Pb [137]. In this experiment the A = 6cm-'
detuning from resonance meant that transparency played little role in the en-
hancement (since the sample was optically thin). However, once the coupling laser
strength satisfied the inequality Slc > ($,opp,er + A2)"2 the dispersion (integrated
across the Doppler profile) became effectively zero, leading to perfect phase
matching and enhanced conversion efficiency.
Other recent work on this topic includes experiments on non-degenerate four-
wave mixing based on E I T in a A scheme in R b [138]. I n this experiment a
coupling field was applied resonantly (w1) whilst a second and third field (w2 and
w p ) were applied at a detuning of 450 MHz. A phase-conjugate field is created at a
+
frequency wc = wl w2 - wp. Measurements were made independently of I m x(')
and x ( ~under
) optically thin conditions, confirming that x ( ~was ) indeed enhanced
by constructive interference. If an optically dense medium was used a significant
enhancement in non-degenerate four-wave mixing was observed. A high phase-
conjugate gain achieved with very low laser powers arising from the presence of
population trapping in a double-A scheme in Na was recently reported [139, 1401.
CW resonant four-wave mixing [141] and frequency up-conversion [142] has been
observed in an experiment investigating a double-A scheme in Na dimers.
494 J. P. Marangos
needs to be populated initially and can remain the only state with significant
population throughout the process. In C P T experiments the concern is primarily
with the changes within the state populations of individual atoms; for E I T the
interest is more especially in the optical response of the entire medium. This optical
response is determined by the coherences rather than by the populations. Within
the language of density matrices for C P T the pertinent measured quantities are
the on-diagonal elements (populations) whilst in E I T they are the off-diagonal
elements (coherences). Most importantly in the limit of a strong-coupling field
( 5 2 2 ) the coherences leading to E I T are almost instantaneously established (on a
time scale of about 1/01, which is typically a few picoseconds). For creation of
population trapping, time scales of several optical pumping times are required
(typically many nanoseconds).
A useful concept that has been used to emphasize the new aspects of these
effects is ‘phaseonium’ [13]. This term summarizes the idea of the formation of a
macroscopic medium consisting of phase-coherent quantum objects (atoms or
molecules). T h e optical properties (both linear and nonlinear) of this (coherent)
medium are very different from those of a normal (incoherent) medium. In these
laser dressed media the language of linear and nonlinear susceptibilities can be
retained only to the extent that it is recognized that all these resonant processes are
highly non-perturbative (i.e. even the ‘linear’ processes involve the coupling of
atoms with many photons). An important consequence of this is that the magni-
tudes of linear and nonlinear susceptibilities can reach equality in a phase-coherent
medium. This is in marked contrast with the normal situation in which the
nonlinear susceptibility is responsible for effects that are many orders of magni-
tude weaker than those arising from the linear susceptibility. As a consequence of
this strong nonlinearity, novel types of pulse propagation (matched pulses) and
high-efficiency frequency up-conversion can occur.
Since 1990 there has been a considerable level of activity devoted to research
into E I T and related topics. This has been motivated by the recognition of a
number of potential new applications, that is lasers without inversion, high-
efficiency nonlinear optical processes, lossless propagation of laser beams through
optically thick media, and high-efficiency population transfer via coherent adia-
batic processes. T h e earlier ideas associated with C P T (first observed in 1976) had
found application mostly as a tool of high-resolution spectroscopy rather than as a
new direction in nonlinear optics. Therefore the concept of E I T has contributed a
distinctive new thrust to work on atomic coherence and its applications.
Although it has been useful for the purposes of this review, for the reasons
stated above, to isolate E I T from other related processes it cannot be ignored that
some of the currently most exciting work on nonlinear optical generation [143,145]
and lossless pulse propagation [54,55] involve two strong laser fields (521 and 5 2 2 )
and the formation of CPT-type states. Therefore we see that it is in the integration
of ideas on atomic coherence, nonlinear optics and laser pulse propagation that
there are likely to be the most interesting future developments.
From the outset an intriguing question is whether E I T effects can be induced
in solid-state media. Experiments have recently been reported that claim to have
observed a modest degree of absorption reduction induced in ruby crystals in
ladder and V configurations using a microwave coupling field applied between
Zeeman shifted components of the ground state with optical frequency probing
[149]. In general the high dephasing rates in solid-state systems will prevent the
496 J . P . Marangos
Acknowledgments
I would like to acknowledge the very useful discussions with Christopher
Dorman, Stephen Harris, Peter Knight and Ulrich Rathe that have guided me in
writing this review. In particular I am indebted to Christoph Keitel for his reading
of the manuscript and his helpful criticism. I would also like to thank Neal Powell
for the preparation of the figures. Despite this invaluable help from colleagues, I
do of course accept full responsibility for any shortcomings, errors or omissions in
this work. This work was supported b y the U K Engineering and Physical Science
Research Council.
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