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OPTICS Copyright © 2024 The

Authors, some rights
Attosecond electron microscopy and diffraction reserved; exclusive
licensee American
Association for the
Dandan Hui†, Husain Alqattan†, Mohamed Sennary, Nikolay V. Golubev, Mohammed Th. Hassan* Advancement of
Science. No claim to
Advances in attosecond spectroscopy have enabled tracing and controlling the electron motion dynamics in original U.S.
matter, although they have yielded insufficient information about the electron dynamic in the space domain. Government Works.
Hence, ultrafast electron and x-­ray imaging tools have been developed to image the ultrafast dynamics of mat- Distributed under a
ter in real time and space. The cutting-­edge temporal resolution of these imaging tools is on the order of a few Creative Commons
tens to a hundred femtoseconds, limiting imaging to the atomic dynamics and leaving electron motion imaging Attribution License 4.0
out of reach. Here, we obtained the attosecond temporal resolution in the transmission electron microscope, (CC BY).
which we coined “attomicroscopy.” We demonstrated this resolution by the attosecond diffraction measure-
ments of the field-­driven electron dynamics in graphene. This attosecond imaging tool would provide more in-
sights into electron motion and directly connect it to the structural dynamics of matter in real-­time and space
domains, opening the door for long-­anticipated real-­life attosecond science applications in quantum physics,
chemistry, and biology.

INTRODUCTION the electrons inside the microscope by ultrashort laser pulses in the

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The advancement in ultrafast science opened a window to see the time domain. This enhancement opened the door to image the col-
ultrafast dynamics of matter span from the material phase transi- lective electron dynamics, such as surface plasmon electron dy-
tions, molecular, atomic, and electronic motions in real time (1–8). namics (41). However, imaging the electron motion requires an
This capability has been extended to include the space dimensions enhancement of the UEM temporal resolution to the subfemtosec-
by developing ultrafast x-­ray and electron imaging tools (9–11). Ul- ond time scale. A train of attosecond electron pulses has been dem-
trafast electron microscopy (UEM) is one of these crucial tools to onstrated in UEM using the gating approach by continuous and
envisage the evolution of the matter dynamics in the four dimen- pulsed laser beams by other groups (32, 36, 37, 42, 43). This train of
sions of space and time (12–16). The basic idea of UEM depends on attosecond electron pulses contains (n) number of electron pulses.
generating ultrafast bursts of electrons inside the microscope by Hence, using this pulse train of electrons in time-­resolved ultrafast
laser pulses to image the matter’s dynamics triggered by another imaging measurement, the dynamical process will be probed (n)
pump laser pulse via time-­resolved measurements (17, 18). Hence, times at every single triggering (pumping) event. Accordingly, the
the imaging temporal resolution is defined by the temporal duration recorded snapshots form a video of the average dynamics (42, 43),
of the electron pulses, not the mechanical shatter of the micro- not as it evolves in time. In this case, the temporal resolution of the
scope detector. UEM remains the same as the temporal profile of the entire train of
At the beginning of the century, the first demonstration of UEM pulses, which lasts a few hundred femtoseconds to infinite when a
with nanosecond resolution was reported to image the laser-­ continuous wave gating laser is used (42, 43). Therefore, the train
induced melting of nickel metal and the morphology change of of attosecond electron pulses is constrained to imaging periodic
cobalt bulk (17). After this pioneer work, many research efforts dynamics, such as the repeatable oscillation of scattered light (42,
were focused on enhancing the temporal resolution of UEM. In 43). However, to resolve nonperiodic attosecond dynamics, such as
2008, the temporal resolution of UEM was enhanced to a subpico- charge migration, electron-­based phase transition, and electronic
second time scale, extending the capability of UEM to image faster motion in the solid-­state system presented in this work, a single
laser-­induced molecular and atomic motions (18). Although fur- attosecond electron pulse (to confine the probing to a single event)
ther enhancement of the UEM temporal resolution was technically must be generated and used inside the microscope.
challenging due to the crucial space charge effect because of travel- In this work, we generate a single attosecond electron pulse by
ing the ultrafast electron wave packet inside the microscope from the optical gating approach using a polarization-­gated half-­cycle la-
the source to the sample. Hence, many research efforts focused on ser pulse (31, 44, 45). Then, we demonstrate the attained attosecond
compressing the electron pulses (19–37) and developing high-­ temporal resolution by measuring the attosecond electron diffrac-
bright photoemission electron sources, such as laser-­driven Schott- tion to probe the sub-­half-­cycle field-­driven electron dynamics of
ky field emission and cold field-­emission guns using the apex of the multilayer single crystalline graphene (fig. S1). We studied these
nanoemitter to generate a few hundred femtoseconds high-­bright electron dynamics theoretically and calculated their effect on chang-
electron pulses (38, 39). Then, the optical-­gating approach has ing the scattered electron intensity. Then, we compare the simula-
been demonstrated to enhance the temporal resolution of UEM by tion results with our attosecond electron diffraction measurements,
an order of magnitude to a few tens of femtoseconds (31, 40). This which show good agreement. The ability to resolve this subcycle
technique is based on controlling the temporal profile and gating dynamics demonstrates the attosecond resolution in the electron
microscope and establishes what we coined “attomicroscopy.” The
attosecond imaging introduced in this work enables the study of the
attosecond electron dynamics of matter and opens the door for a
Department of Physics, University of Arizona, Tucson, AZ 85721, USA.
*Corresponding author. Email: mohammedhassan@​arizona.​edu variety of attosecond imaging applications. Moreover, this long-­
†These authors contributed equally to this work. awaited imaging of electron motion in action can reveal electron

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S c i e n c e A d v a n c e s | R e s e ar c h R e s o u r c e

dynamics in complex and quantum systems and promises to break frequency response (46). The OGP beam (beam diameter, ~200 μm)
new ground in physics, chemistry, biochemistry, and biology. is directed to the aluminum grid as illustrated in Fig. 2A. The angle
between the electron and the OGP beams is <2° (see fig. S2B). The
electron and OGP pulses are traveling at different speeds, so no in-
RESULTS AND DISCUSSION teraction occurs before the gating medium. Second, the OGP inter-
In our attosecond electron microscopy setup (Fig. 1A), the acts with the gating medium and induces an evanescent scattered
polarization-­gated half-­cycle laser pulse has been generated using light field, which has a comparable speed and interacts with the
the polarization gating (PG) method (see the basic principle in main electron pulse. The electrons couple efficiently with the lin-
Fig. 1B and the setup in fig. S2A). This pulse is used as an optical early polarized part of the scattered field [the interaction with the
gating pulse (OGP) to gate and generate the single attosecond elec- circularly polarized sides of the field is minimal due to the averag-
tron pulses inside the microscope by the optical gating approach, ing out of these parts (41)] and exchange momentum. Then, some
which can be explained as follows: First, the main ultrafast electron of these electrons gain or lose (n) number of photons from the scat-
pulse (a few hundred femtoseconds duration) propagates from the tered field. Hence, these electrons are gated in a temporal window
photocathode to the transmission electron microscope (TEM) similar to the duration of the linearly polarized half-­cycle of the
dense-­mesh aluminum grid (thickness = 20 ±3 μm and pitch size is OGP (625 as) to generate a single-­attosecond electron pulse. The
83 μm) placed on the top of the sample (see Fig. 2A), which acts generated attosecond electron pulse in our approach is generated
as a gating medium. We opted to use aluminum due to its broad on the Al grid just on top of the sample, so the space charge effect

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Attosecond electron microscope

First arm UV laser pulse

Ultrafast
SHG Lens mirror electron pulse

Delay
stage Pump laser pulse
Second arm

Optical gating Al gating grid

Beam pulse (OGP)
splitters Sample

B Polarization gating of laser pulse

625 as
Gated electron
0° pulse
45°
Optical gating
Zero-order pulse (OGP)
waveplate t0
Multiple-order t1
waveplate t2
t3

Fig. 1. Attosecond electron microscope setup. (A) The setup consists of two arms; the first arm is an NIR laser pulse propagating through a second-­harmonic generation
(SHG) crystal to generate a UV laser pulse. This UV beam is directed to the photocathode inside the microscope to emit ultrafast electron pulses. In the second arm, a 5-­fs
laser pulse is divided by a beamsplitter into two beams. The first beam is reflected off two mirrors mounted on a nanometer-­precision delay stage and is sent to the mi-
croscope. This beam is used as the pump pulse to trigger the electron motion in the system under study. The second beam undergoes the PG process, which is illustrated
in (B). In this process, the input linearly polarized laser pulse passes through multi-­order and zero-­order waveplates set at 45° and 0°, respectively. The generated pulse has
a half-­cycle linear-­polarized field in the middle and a circularly polarized field at the edges. This pulse is used as an optical gating pulse (OGP) of the electrons inside the
microscope. The OGP beam is directed to the sample position where the electron gating and the generation of the attosecond electron pulses take place. These gated
electrons can be used to record images (diffraction/direct) to probe the electron dynamics of matter.

Hui et al., Sci. Adv. 10, eadp5805 (2024) 21 August 2024 2 of 8

S c i e n c e A d v a n c e s | R e s e ar c h R e s o u r c e

A 1

Electric field (arb. unit)

A Pump B 1st -order Bragg diffraction peaks
pulse 2nd -order Bragg diffraction peaks
OGP 3rd -order Bragg diffraction peaks
Gating Al 0

medium
-1
-9 -6 -3 0 3 6 9
Time (fs)

B C D

fs fs fs
.4 .2
Gated Sample =
-7
=
-2
=
-1
electrons 3 33 33 3
Ungated K -1 ) K -1 ) K -1 )
(n 0 0 m (n 0 0 m (n 0 0 m
electrons
y y y
m- (n m- (n m- (n
)1 KX )1 KX )1 KX
E -3 -3 F -3 -3 G -3 -3 1
Fig. 2. Optical gating of electron pulse. (A) Illustration of the electron and laser 0.5
fs
pulse interaction on the gating medium (aluminum grid) above the sample of gra- fs 4 fs
0 2. 9 0
phene. (B) Measured diffraction pattern of the multilayer graphene sample. = = =
3 33 33 3
K -1 ) K -1 ) K -1 )
y (n 0 0 m y (n 0 0 m y (n 0 0 m
does not substantially affect the gated electron pulse duration. The m- (n m- (n m- (n
)1 KX )1 KX )1 KX

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number of gated electrons is estimated to be 0.1% of the total num- -3 -3 -3 -3 -3 -3
ber of electrons (~106 electrons/s) generated from the photocath-
Fig. 3. Light field–induced electron dynamics in the reciprocal space of gra-
ode, which is sufficient to probe and image the ultrafast electron phene. (A) The measured waveform of the pump pulse which is used in the theo-
motion dynamics, enhancing the temporal resolution of the TEM retical calculations and diffraction measurements. (B to G) Snapshots of the EDD in
to the subfemtosecond time scale. As a proof-­of-­principle of the ob- the reciprocal space of graphene at different time instants (indicated by dashed
tained attosecond resolution, the subfemtosecond gated electrons gray lines in (A) in the presence of and after the end of the driver field. Each snap-
are used to image the sub-­half-­cycle field-­driven electron motion shot is normalized with respect to the snapshot in (G) for better visualizing of the
dynamics triggered by the pump pulse (field strength = 2.5 V/nm) EDD (the normalization factor is mentioned in the right side inset).
in a single-­crystal multilayer graphene sample (sample preparation
is explained in the Supplementary Materials) by attosecond time-­
resolved electron diffraction measurements (diffraction pattern of
graphene is shown in Fig. 2B). bands, D(kt) is the matrix of transition dipole moments, the com-
Before we discuss our attosecond diffraction experiment results, mutator symbol “{}” is defined as {A, B} = AB − BA, and Td is the
we performed a theoretical study to understand the electron motion interband dephasing time. The required energies of the bands Ei(k)
dynamics in graphene. In a strong light field, there are two induced and the transition dipole moments D(k) were obtained by employ-
electron dynamics: (i) the interband dynamics caused by the popu- ing the nearest-­neighbor tight-­binding model of M-­layer (M = 6 in
lation transfer between the valence band (VB) and conduction band our simulations) AB-­stacked graphene.
(CB) and the related coherent dynamics, and (ii) the intraband dy- The simulations are performed in the time-­dependent crystal
namics generated due to the electron motion within the bands (47). momentum frame, which evolves according to the Bloch accelera-
These field-­driven dynamics follow the waveform of the pump pulse tion theorem
and occur in a sub-­half-­cycle time scale. Accordingly, it was crucial k t = k + e∕ℏ A(t) (2)
to measure our pump waveform using the all-­optical light field sam-
pling methodology we established elsewhere (7, 8, 48). The sampled where k is the wave vector of the field-­free electron and the interac-
field is shown in Fig. 3A. Accordingly, in our presented theoretical tion with the applied electric field E(t) (Fig. 3A) is( governed by the
corresponding vector potential A(t) = − ∫−∞ dt � E t � . We assumed
t )
study, we used the same parameters of the experiment and the mea-
sured pump pulse waveform. the applied electric field is linearly polarized along the C-­C bonds of
Our theoretical study is based on quantum-­mechanical simula- the graphene sample and has a peak strength of 2.5 V/nm.
tions of the field-­induced electron motion dynamics in multilayer At the initial moment of time t0, the electron density occupies the
graphene. It is composed of two main parts: lowest energy electronic state, so that ρ1,1(k, t0) = 1 and ρm,m(k, t0) =
In the first part, we calculated the evolution of the electron den- 0 for m > 1. The action of the laser field leads to the population
sity distribution (EDD) in reciprocal space by solving the Bloch transfer from the ground state to the excited electronic states of the
equation (49, 50) system, which is reflected in the changes of the matrix elements
𝜕 ( ( ) ( )) of the density matrix ρ(k, t). The evolution of the matrix element
iℏ ρm,n (k, t) = Em k t − En k t ρm,n (k, t) +
𝜕t ρ12,12(k, t), which represents the part of the electron density occupy-
{ ( ) } 1 − δm,n (1) ing the highest electronic state (reciprocal space) of six-­layer gra-
E(t) ⋅ D k t , ρ(k, t) m,n − i ρm,n (k, t) phene. The rate of the population transfer for given parameters of
Td the applied field at the specific point in reciprocal space is defined by
where E(t) is the applied electric field, ρm,n(k, t) denotes the matrix the transition dipole moments connecting the electronic states but
element of the density matrix ρ(k, t), Ei(kt) are the energies of the also depends on the energy gaps between the corresponding states

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S c i e n c e A d v a n c e s | R e s e ar c h R e s o u r c e

(see Eq. 1). The reciprocal lattice of graphene represents a hexagonal where SBZ denotes the area of the Brillouin zone, and Ψn (k, r) =
pattern with two inequivalent and high-­symmetry points K and K′, ∑
2M

referred to as Dirac points (51). The VB and CB of graphene touch ψ nj (k)Φj (k, r) are the field-­free wave functions of π electrons of
each other at these points, forming the so-­called Dirac cones. While j=1
graphene (in total 12 electronic states for six-­layer graphene). The
the energy gaps in the vicinity of the crossings become small, the
expansion coefficients ψnj(k) are the eigenstates of the tight-­binding
transition dipole moments become large, which make the popula-
Hamiltonian, and Φj(k, r) are the Bloch states of graphene
tion transfer very efficient at the Dirac points. The redistribution of
populations between the bands reflected in the changes of the diago-
nal elements ρm,m(k, t) of the density matrix, also causes the evolution 1 � ik⋅Ri
N
� �
in time of the off-­diagonal elements ρm,n(k, t), which are referred to Φj (k, r) = √ e φ2pz x − Ri (4)
as the electronic coherences. N i=1
The calculated snapshots of the EDD dynamics in the reciprocal
space at different time (τ) instants (as shown in Fig. 3, B to G), where where the summation is made over N atoms in the sublattice, and
the EDD around the Dirac point (Kx = 0 and Ky = 0) is driven by the φ2pz denotes the carbon 2pz atomic orbitals centered at the nuclei
Landau-­Zener (LZ) mechanism dynamics in space (52). Initially, at located at the position Ri.
the arrival of the field (τ = −7 fs), only the excited electrons local- In the second part, we calculated and plotted snapshots of the
ized around the Dirac point are involved in the dynamics, as illus- real space EDD at different time instants in Fig. 4 (a full movie is
trated in Fig. 3B. Then, as the field strength increases at τ = −2.4 fs, provided in movie S2). Note that the carbon atoms of the top gra-
the excited electrons migrate to the positive Kx direction, as depicted phene layer and the bonds between these atoms are shown in solid
in Fig. 3C. At τ = −1.2 fs, the electrons are returned toward the Kx black circles and lines, respectively. Before the field arrival, the elec-
trons are in the equilibrium state, and no EDD change occurs. At the

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negative direction following the field shape, as shown in Fig. 3D. At
the field’s highest half-­cycle strength (τ = 0 fs), the electrons reach maxima of the first half-­cycle (τ = −2.4 fs), the change in the EDD
their largest displacement along Kx axis (see Fig. 3E). The displace- is observable, as shown in Fig. 4A. In this snapshot, the EDD is
ment of electrons towards negative Kx (τ = −1.2 fs, Fig. 3D) and more localized around A, B, and C than A , B , and C atoms. Also, the
positive Kx (τ = 0 fs, Fig. 3C) are not symmetric with respect to the EDD intensities between BB, CC, and AA(from the next unit cell)
Dirac point, indicating that the electron displacement depends on atoms are lower than between AB , AC , BA , and AC atoms in space.
the strength of the driver field. Moreover, the number of excited When the field flips the direction at τ = −1.2 fs (Fig. 4B), the
electrons at the reciprocal space increases, and the EDD spreads in electrons migrate toward the A , B , and C atoms, and the EDD local-
positive and negative directions of Ky. At τ 2.4 fs, the EDD is mini- ization differences between A, B, and C and A , B , and C atoms de-
mal around the Dirac point and more spread in both directions crease. Furthermore, near the field maxima (τ = 0 fs), the EDD
(positive and negative values) of Kx and Ky, as shown in Fig. 3F. After localization difference around and between the atoms is maximized,
the end of the field (at τ = 9 fs); the EDD is all over the reciprocal as illustrated in Fig. 4C. Then, after a half-­cycle (at τ = 1.2 fs), the
space (Fig. 3G). While the populations of the bands remain constant field flips the direction, and the EDD difference around the atoms
after the action of the external field on the system, the electronic becomes smaller as shown in Fig. 4D. At τ = 2.4 fs (the maxima of
coherences are expected to decay rapidly due to the various deco- the third half-­cycle of the field), the localizing difference of the EDD
herence effects, such as temperature fluctuations and the variations increase again, as illustrated in Fig. 4E. Although the EDD between
of the laser field parameters. The full mapping of the electron dy- the carbon atoms in Fig. 4E remains less than in Fig. 4C and higher
namics in the reciprocal space is provided in movie S1. than in Fig. 4A because in this case, the field strength is less than the
The computed reciprocal space density matrix ρ(k, t) provides main half cycle at τ = 0 fs but higher than the field strength of the
access to the real-­space EDD [Q(r, t)], which can be decomposed in first half cycle at τ = −2.4 fs. This indicates that the EDD in real
the noncoherent Qncoh(r, t) and coherent Qcoh(r, t) contributions as space depends on the direction and the strength of the driver field,
following similar to the electron motion in the reciprocal space (Fig. 3, B to G).
Next, we calculated the electron diffraction signal of multilayer
graphene based on the simulated EDD [Q(r, t)] dynamics in real
⎛
⎜ space shown in Fig. 4. Our approach is based on the assumption that
⎜ 2M projectile electrons scatter from the graphene electron density elas-
2 ⎜� � � ��2
SBZ ⎜ m=1 ∫ m,m
Q(r, t) = ρ (k, t)�Ψm k t , t � dk + tically (53), e.g., without causing interference effects (54). We note in
� �
⎜ ������������������������������������������� passing that taking the quantum nature of the scattering process
⎜ into consideration is a notoriously difficult task. Despite the notable
⎝ Qncoh (r,t) (3) efforts in this direction in recent years (54–70), full quantum calcu-
⎞ lations are possible only for atoms and small molecules under cer-
⎟ tain assumptions, while no such calculations for electron dynamics
�
2M
� � � � �� ⎟ in solid-­state systems have been reported so far.
∫
2 Re ρm,n (k, t)Ψ∗m k t , r Ψn k t , r dk ⎟ In the first-­Born approximation, the intensity of the scattered
m>n
⎟
�������������������������������������������������������������������⎟ electron beams from a periodic solid is given by (71)
⎟
Qcoh (r,t) ⎠
1 || |2
2|∫
IG (t) ∝ Q(r, t)exp(iG ⋅ r)dr || (5)
G | unit cell |

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S c i e n c e A d v a n c e s | R e s e ar c h R e s o u r c e

A = -2.4 fs B = -1.2 fs C = 0 fs D = 1.2 fs E = 2.4 fs

1
2
B B
1 0

Y (Å)
0 A A
A
-1
-1 C C
-2
-2 -1 0 1 2 -2 -1 0 1 2 -2 -1 0 1 2 -2 -1 0 1 2 -2 -1 0 1 2
X (Å)
Fig. 4. Graphene electron motion dynamics in real space. (A to E) Calculated snapshots of the field-­induced electron motion at different time instants. These snapshots
show the change in the EDD around and between the carbon atoms of graphene at different time instants in real space. The red, blue, and white colors represent the high
(positive), low (negative), and zero values of the EDD, respectively.

where the integration is performed in the unit cell and G is recipro- modulating as a function of time, respectively. Please note that the
cal lattice vector. Assuming a perpendicular orientation of the gra- gated electrons have subfemtosecond resolution, while the ungated
phene sample with respect
� � to�the incoming
� electron
�� beam and using electron temporal resolution remains a few hundred femtoseconds.
the fact that G = 2π p 1 1
√ , 1 + q √ , − 1 for graphene (51), we So, the intensity modulation signature is carried only on the gated
a 3 3 electrons, while the ungated electron remains unchanged. Accord-
can integrate Eq. 5 along z axis explicitly thus obtaining ingly, this scattered gated electron intensity modulation is retrieved

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by subtracting the dark diffraction pattern (at τ ≤ −9 fs) and the
3a2 ungated electrons (background), as explained in the Supplementary
Ip,q (t) ∝ � �
16 p2 − pq + q2 π2 Materials. The measured and simulated diffraction change of gra-
� � � �� �2 phene dynamics triggered by strong field (Fig. 5, A to C) are in ac-
� � � 1 � � � � �
�∫
� 2π ceptable agreement.
Q x, y, t exp i √ p+q x + p−q y dxdy��
� unit cell a 3 � Next, to confirm that the main cause for the scattering electron
� �
intensity change is the electron motion within the CB as explained
(6)
earlier, we calculated the intraband
where Q(x, y, t) = ∫ Q(r, t)dz is the electron density integrated over
z direction and p and q are Miller indices. The obtained Bragg spots ∑
2M
( )
∫
diffraction intensities Ip,q(t) are averaged in each order and convo- J intra (t) ∝ ρm,m (k, t)∇k Em k t dk (8)
luted with a Gaussian function to account for a finite duration of the m=1

incident electron beam and interband band

+∞ � � ∑
2M
{ ( ( ) ( )) ( )}
(τ − t)2 �
∫ σ 2π ∫
̃I BZ (t) = 1 J inter (t) ∝ 2 Im ρm,n (k, t) Em k t − En k t Dn,m k t dk
√ exp − I (τ) dτ (7)
2σ2 p,q ∈ BZ p,q m>n
−∞
(9)
currents and fitted them to the measured diffraction intensity mod-
where the summation is performed over all combinations of indices ulations. The fitted curves [plotted in the red line in Fig. 5 (A to C)]
belonging to a corresponding order, and parameter σ = FWHM
√ char- follow the main diffraction intensity oscillations of the first-­, sec-
σ 2π
acterizes the width of the electron pulse. The calculated scattered ond-­, and third-­order peaks. The small deviation on the sides may
intensity changes for the first, second and third Bragg diffraction be attributed to the underestimation of the dispersion effect experi-
peaks are shown in blue color in Fig. 5 (A to C, respectively). enced by the pump field with respect to the sample position in the
The change in the scattered electron intensity is attributed to the performed field sampling measurement.
displacement of the EDD between the carbon atoms in real space The fitting results show that the contribution of the intraband
(Fig. 4), which is caused mainly by intraband dynamics. While the current is more substantial (estimated to be ~87, ~85, and ~80% for
EDD change due to the interband dynamics is localized around each the first, second, and third diffraction peaks’ dynamics, respectively)
carbon atom and occurs in the same direction as the incident elec- than the interband current.
tron beam. Hence, the interband transition can barely affect the The resolution of the half-­cycle electron diffraction modulations
scattering electron intensity. in the diffraction measurements presented in Fig. 5 (A to C) vali-
In our experiment, the electron diffraction pattern of graphene dates the attained attosecond imaging resolution.
(Fig. 2B) is recorded as a function of the time delay (with a time step Although our microscope is not equipped with an energy ana-
size of 300 as) between the OGP (gated electron pulses) and the lyzer and spectrometer to directly separate and measure the gated
pump pulses. Note the OGP is set at a low value of ~0.85 V/nm to pulse duration, but we performed a few additional experiments to
ensure that it is not triggering the graphene electron dynamics. confirm the achieved attosecond resolution, which is the main goal
The retrieved time-­resolved attosecond electron diffraction re- of this work. First, after recording the measurements presented in
sults show that the intensity of the first-­, second-­, and third-­order Fig. 5, we reduced the pump field strength to <2 V/nm (low-­field
scattered diffraction peaks, presented in black dots connected with regime) (47). The electron diffraction intensity modulation disap-
dashed black lines (average of seven scans) in Fig. 5 (A to C), are peared, indicating that the measured signal is due to graphene’s

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S c i e n c e A d v a n c e s | R e s e ar c h R e s o u r c e

4 A Calculated electron scattering intenisty

Electron current
1st-order Bragg diffraction peaks long-­standing challenges in ultrafast time-­resolved electron imag-
Change of the scattering intenisty (arb. unit)

0.5 ing measurements in UEM and ultrafast electron diffraction (UED).

0 This work demonstrates the attosecond temporal resolution, ob-
0
-4 -0.5
tained by attosecond optical gating, inside TEM. Moreover, we per-
formed attosecond electron diffraction imaging to study the electron

Electron current (arb. unit)

5 B 2nd-order Bragg diffraction peaks dynamics of matter. Our results show a strong correlation between
1
field-­induced electron dynamics in the CB and the real space elec-
0 tron motion between the carbon atoms in graphene. This work
0
-5
paves the way for recording images of electron motion in the four
-1 dimensions of space and time and opens a window to see the quan-
10 C
3rd -order Bragg diffraction peaks
1 tum world in real systems and answer fundamental questions in
physics. Moreover, the capability of attosecond electron microscope
0 0 imaging to connect the light-­induced electron dynamics and the
-10 morphology of matter in real-­space builds the desired bridge be-
-1
tween science and technology to engineer petahertz and quantum
-9 -6 -3 0 3 6 9 12 15
Delay (fs)
photonics (72, 73). Furthermore, electron imaging would allow
filming and controlling the chemical and biochemical reactions in
Fig. 5. Attosecond electron diffraction of graphene. (A to C) The measured aver- real time, which would advance the fields of material synthesis, drug
age scattering intensity changes of the first-­, second-­, and third-­order diffraction design, and personalized medicine to the next level.
peaks as they evolve in time are shown as black dots connected with dashed black

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lines, respectively. The error bars present the SD uncertainty of the relative scat-
tered peak intensity of seven scans. The calculated diffraction intensity oscillations, MATERIALS AND METHODS
caused by the field-­induced electron motion in real space, are plotted in a solid In our setup (Fig. 1A), a 1-­mJ laser pulse (16 fs) centered at 750 nm
blue line, while the fitted field-­induced electron current is plotted in a solid red line.
is generated from an optical parametric chirped-­pulse amplification–
based (passively carrier-­envelope phase stabilized) laser system
with a 20-­kHz repetition rate. The beam is divided into two beams
strong field-­driven electron dynamics (see fig. S3). In addition, this by a 10:90 beamsplitter. Each beam is sent to one arm of the setup.
result excludes the possibility that the measured diffraction change In the first arm, the 10% (~2 W) portion of the main laser beam is
is increased due to any interference effect between the pump and the sent to a second-­harmonic generation (SHG) unit to generate an
gating laser pulses. We observed the scattering intensity modulation ultraviolet beam (λ = 380 nm). The ultraviolet beam is focused
signal again by ramping up the power of the pump pulse back to the onto a photocathode inside the microscope to generate the main
high field strength of 2.6 V/nm. ultrafast electron pulses (typically having a duration of a few hun-
In a second confirmation experiment, we blocked the OGP and dred femtoseconds). The UV beam is kept at the lowest power to
repeated the electron diffraction measurements. The measured dif- minimize the number of electrons per pulse and the related space-­
fraction patterns showed no intensity change in the Bragg spots (at charge effect. Then, these electrons are accelerated to 200 keV and
any order) in the time window between −10 and 15 fs, as expected focused by the magnetic lenses into the sample understudy inside
(see fig. S4). In this case, the electron imaging resolution is defined the microscope.
by the main electron pulse from the photocathode (no gated elec- In the second arm, 90% of the main laser beam is focused on a
trons), which is on the order of a few hundred femtoseconds. Then, hollow-­core fiber filled with neon gas under 2.5-­bar pressure using a
we released the OGP to gate the electrons again on the sample and 1-­m lens. The beam undergoes a strong nonlinear propagation and
repeated the time-­resolved diffraction measurement under the same generates a broadband spectrum that spans over 250 to 1000 nm.
conditions. The intensity oscillations of the diffraction peaks were The power of the supercontinuum after the fiber is 4 W (200 μJ).
observed again. Last, we performed the experiment under the same This supercontinuum enters a chirp mirror compressor (optimized
conditions but with the gating medium (aluminum grid) removed. to compress a broadband spectrum from 400 to 1000 nm) to gener-
The results show no resolved oscillations (see fig. S5), confirming ate a Fourier-­limited 5-­fs laser pulse (p-­polarized). Note that the
the measured diffraction results in Fig. 5 (A to C) occurred due compressor precompensates for the pulse dispersion due to the
to the generation of the subfemtosecond gated electron pulse at the propagation through the dispersive elements [waveplates, windows,
aluminum grid. neutral density (ND) filters, etc.] in the beam path until the pulse
Notable, many experimental factors are vital for performing the reaches the sample inside the microscope. The beam exits the com-
presented attosecond electron imaging experiment, such as (i) the pressor and enters the PG unit to generate a polarization-­gated laser
high repetition rate of the laser, which allows the gating of a high pulse (fig. S2A). The 5-­fs (p-­polarized) laser pulse is divided into
number of electrons, (ii) the high stability of the laser beam inten- two beams via a 30:70 beam splitter (BS#1). The transmitted beam
sity (root mean square = 0.3%), which allows us to achieve a low carries 70% of the beam power and acts as the “pump” pulse to trig-
noise level of the electron intensity fluctuation in the microscope, ger the ultrafast electron dynamics of the sample. This pump beam
and (iii) the low jitter between the gated electrons (controlled by the also passes through an ND to control the pump pulse field strength.
OGP pulse) and laser pump pulses, which is measured and deter- The reflected beam (carries 30% of the beam power) is acting as the
mined during our measurements to be in the range of ~100 as. This OGP. This beam passes through another ND filter to control the
inherited extremely low jitter is one of the notable features of the OGP power. Then, the beam passes through a multi-­order wave-
demonstrated optical gating approach, which overcomes one of the plate. Hence, the output beam contains p-­polarized and s-­polarized

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S c i e n c e A d v a n c e s | R e s e ar c h R e s o u r c e

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57. H.-­C. Shao, A. F. Starace, Imaging coherent electronic motion in atoms by ultrafast and/or the Supplementary Materials.
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58. H.-­C. Shao, A. F. Starace, Imaging electronic motions in atoms by energy-­resolved Submitted 9 April 2024
ultrafast electron diffraction. Phys. Rev. A 90, 032710 (2014). Accepted 19 July 2024
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