Electron Wave Packet Research Articles

Spatiotemporal Electron Beam Focusing through Parallel Interactions with Shaped Optical Fields.

The ability to modulate free electrons with light has emerged as a powerful tool to produce attosecond electron wave packets. However, research has so far aimed at the manipulation of the longitudinal wave function component, while the transverse degrees of freedom have primarily been utilized for spatial rather than temporal shaping. Here, we show that the coherent superposition of parallel light-electron interactions in transversally separate zones allows for a simultaneous spatial and temporal compression of a convergent electron wave function, enabling the formation of sub-Ångström focal spots of attosecond duration. Specifically, spots spanning just ∼3% of the light optical cycle are shown to be formed, accompanied by an increase by only a factor of 2 in spatial extension relative to an unperturbed beam. The proposed approach will facilitate the exploration of previously inaccessible ultrafast atomic-scale phenomena, in particular enabling attosecond scanning transmission electron microscopy.

Ultrafast Coupling of Optical Near Fields to Low-Energy Electrons Probed in a Point-Projection Microscope.

We report the first observation of the coupling of strong optical near fields to wavepackets of free, 100 eV electrons with <50 fs temporal resolution in an ultrafast point-projection microscope. Optical near fields are created by excitation of a thin, nanometer-sized Yagi-Uda antenna, with 20 fs near-infrared laser pulses. Phase matching between electrons and near fields is achieved due to strong spatial confinement of the antenna near field. Energy-resolved projection images of the antenna are recorded in an optical pump-electron probe scheme. We show that the phase modulation of the electron by transverse-field components results in a transient electron deflection while longitudinal near-field components broaden the kinetic energy distribution. This low-energy electron near-field coupling is used here to characterize the chirp of the ultrafast electron wavepackets, acquired upon propagation from the electron emitter to the sample. Our results bring direct mapping of different vectorial components of highly localized optical near fields into reach.

Nondipole signatures in ionization and high-order harmonic generation

We analyze nondipole effects arising in ionization and high-order harmonic generation for a two-dimensional hydrogen atom irradiated with either low- or high-frequency laser pulses. In the low-frequency case, the electron wave packet dynamics is dominated by rescattering processes within the laser pulse. Here both odd- and even-order harmonics are generated in the direction of the laser field propagation and polarization, respectively. For high-frequency pulses, such rescattering processes can be neglected. We demonstrate that a significant portion of photoelectrons is detected opposite to the laser pulse propagation direction as a consequence of their postpulse wave packet spreading and interaction with the parent ion. This is accompanied by rich interference structures formed in the momentum distributions of photoelectrons. Our results follow from the numerical solution of the time-dependent Schr\"odinger equation, which is based on the Suzuki-Trotter scheme with the split-step Fourier approach. The method relies on a Hamiltonian decomposition, where except for the components depending exclusively on the momentum or on the position operators, there are also terms depending on both momentum and position operators in particular configurations. We demonstrate that, as long as the latter does not depend on noncommuting coordinates of the momentum and position operators, nondipole effects in laser-matter interactions can be studied without applying extra approximations and unitary operations.

Attosecond Real-Time Observation of Recolliding Electron Trajectories in Helium at Low Laser Intensities.

Laser-driven recollision physics is typically accessible only at field intensities high enough for tunnel ionization. Using an extreme ultraviolet pulse for ionization and a near-infrared (NIR) pulse for driving of the electron wave packet lifts this limitation. This allows us to study recollisions for a broad range of NIR intensities with transient absorption spectroscopy, making use of the reconstruction of the time-dependent dipole moment. Comparing recollision dynamics with linear vs circular NIR polarization, we find a parameter space, where the latter favors recollisions, providing evidence for the so far only theoretically predicted recolliding periodic orbits.

Projectile Coherence Effects in Twisted Electron Ionization of Helium

Over the last decade, it has become clear that for heavy ion projectiles, the projectile’s transverse coherence length must be considered in theoretical models. While traditional scattering theory often assumes that the projectile has an infinite coherence length, many studies have demonstrated that the effect of projectile coherence cannot be ignored, even when the projectile-target interaction is within the perturbative regime. This has led to a surge in studies that examine the effects of the projectile’s coherence length. Heavy-ion collisions are particularly well-suited to this because the projectile’s momentum can be large, leading to a small deBroglie wavelength. In contrast, electron projectiles that have larger deBroglie wavelengths and coherence effects can usually be safely ignored. However, the recent demonstration of sculpted electron wave packets opens the door to studying projectile coherence effects in electron-impact collisions. We report here theoretical triple differential cross-sections (TDCSs) for the electron-impact ionization of helium using Bessel and Laguerre-Gauss projectiles. We show that the projectile’s transverse coherence length affects the shape and magnitude of the TDCSs and that the atomic target’s position within the projectile beam plays a significant role in the probability of ionization. We also demonstrate that projectiles with large coherence lengths result in cross-sections that more closely resemble their fully coherent counterparts.

High resolution metrology of autoionizing states through Raman interferences

Metrology of electron wavepackets is often conducted with the technique of photoelectron interferometry. However, the ultrashort light pulses employed in this method place a limit on the energy resolution. Here, weadvance ultrafast photoelectron interferometry access both high temporal and spectral resolution. The key to our approach lies in stimulating Raman interferences with a probe pulse and while monitoring the modification of the autoionizing electron yield in a separate delayed detection step. As a proof of the principle, we demonstrated this technique to obtain the components of an autoionizing nf′ wavepacket between the spin-orbit split ionization thresholds in argon. We extracted the amplitudes and phases from the interferogram and compared the experimental results with second-order perturbation theory calculations. This high resolution probing and metrology of electron dynamics opens the path for study of molecular wavepackets.

Tracing attosecond electron emission from a nanometric metal tip.

Solids exposed to intense electric fields release electrons through tunnelling. This fundamental quantum process lies at the heart of various applications, ranging from high brightness electron sources in d.c. operation1,2 to petahertz vacuum electronics in laser-driven operation3-8. In the latter process, the electron wavepacket undergoes semiclassical dynamics9,10 in the strong oscillating laser field, similar to strong-field and attosecond physics in the gas phase11,12. There, the subcycle electron dynamics has been determined with a stunning precision of tens of attoseconds13-15, but at solids the quantum dynamics including the emission time window has so far not been measured. Here we show that two-colour modulation spectroscopy of backscattering electrons16 uncovers the suboptical-cycle strong-field emission dynamics from nanostructures, with attosecond precision. In our experiment, photoelectron spectra of electrons emitted from a sharp metallic tip are measured as function of the relative phase between the two colours. Projecting the solution of the time-dependent Schrödinger equation onto classical trajectories relates phase-dependent signatures in the spectra to the emission dynamics and yields an emission duration of 710 ± 30 attoseconds by matching the quantum model to the experiment. Our results open the door to the quantitative timing and precise active control of strong-field photoemission from solid state and other systems and have direct ramifications for diverse fields such as ultrafast electron sources17, quantum degeneracy studies and sub-Poissonian electron beams18-21, nanoplasmonics22 and petahertz electronics23.

Periodic electron oscillation in coupled two-dimensional lattices

We study the time evolution of electron wavepacket in the coupled two-dimensional (2D) lattices with mirror symmetry, utilizing the tight-binding Hamiltonian framework. We show analytically that the wavepacket of an electron initially located on one atomic layer in the coupled 2D square lattices exhibits a periodic oscillation in both the transverse and longitudinal directions. The frequency of this oscillation is determined by the strength of the interlayer hopping. Additionally, we provide numerical evidence that a damped periodic oscillation occurs in the coupled 2D disordered lattices with degree of disorder W, with the decay time being inversely proportional to the square of W and the frequency change being proportional to the square of W, which is similar to the case in the coupled 1D disordered lattices. Our numerical results further confirm that the periodic and damped periodic electron oscillations are universal, independent of lattice geometry, as demonstrated in AA-stacked bilayer and tri-layer graphene systems. Unlike the Bloch oscillation driven by electric fields, the periodic oscillation induced by interlayer coupling does not require the application of an electric field, has an ultrafast periodicity much shorter than the electron decoherence time in real materials, and can be tuned by adjusting the interlayer coupling. Our findings pave the way for future observation of periodic electron oscillation in material systems at the atomic scale.

Microscopic Quantum Transport Processes of Out‐of‐Plane Charge Flow in 2D Semiconductors Analyzed by a Fowler–Nordheim Tunneling Probe

AbstractWeak interlayer couplings at 2D van der Waals (vdW) interfaces fundamentally distinguish out‐of‐plane charge flow, the information carrier in vdW‐assembled vertical electronic and optical devices, from the in‐plane band transport processes. Here, the out‐of‐plane charge transport behavior in 2D vdW semiconducting transition metal dichalcogenides (SCTMD) is reported. The measurements demonstrate that, in the high electric field regime, especially at low temperatures, either electron or hole carrier Fowler–Nordheim (FN) tunneling becomes the dominant quantum transport process in ultrathin SCTMDs, down to monolayers. For few‐layer SCTMDs, sequential layer‐by‐layer FN tunneling is observed to dominate the charge flow, thus serving as a material characterization probe for addressing the Fermi level positions and the layer numbers of the SCTMD films. Furthermore, it is shown that the physical confinement of the electron or hole carrier wave packets inside the sub‐nm thick semiconducting layers reduces the vertical quantum tunneling probability, leading to an enhanced effective mass of tunneling carriers.

Waveform Modulation of High-Order Harmonics Generated from an Atom Irradiated by a Laser Pulse and a Weak Orthogonal Electrostatic Field

The detailed characteristics of the harmonics emission of atoms driven via a linearly polarized laser field combined with an orthogonal, weaker electrostatic field were investigated by numerically solving the time-dependent Schrödinger equation. It was found that the direction of the laser polarization and the polarization of the attosecond light, which is synthesized from the harmonic, can be controlled by the amplitude of the electrostatic field. With the analysis of the spatial distribution of the time-dependent dipole moment and the time-dependent evolution of the electronic wave packet, the control mechanism for the harmonic characters was investigated. The generation of harmonics in the vertical direction of the laser electric field is caused by the breaking of the symmetry of the time wave packet distribution. With this mechanism, we obtained circularly polarized attosecond light.

Collision of two interacting electrons on a mesoscopic beam splitter: Exact solution in the classical limit

Experiments on collisions of isolated electrons guided along the edges in quantum Hall setups can mimic mixing of photons with the important distinction that electrons are charged fermions. In the so-called electronic Hong-Ou-Mandel (HOM) setup uncorrelated pairs of electrons are injected towards a beamsplitter. If the two electron wave packets were identical, Fermi statistics would force the electrons to scatter to different detectors, yet this quantum antibunching may be confounded by Coulomb repulsion. Here we model an electronic HOM experiment using a quadratic 2D saddle point potential for the beamsplitter and unscreened Coulomb interaction between the two injected electrons subjected to a strong out-of-plane magnetic field. We show that classical equations of motion for the drift dynamics of electrons' guiding centers take on the form of Hamilton equations for canonically conjugated variables subject to the saddle point potential and the Coulomb potential where the dynamics of the center-of-mass coordinate and the relative coordinate separate. We use these equations to determine collision outcomes in terms of a few experimentally tuneable parameters: the initial energies of the uncorrelated electrons, relative time delay of injection and the shape of the saddle point potential. A universal phase diagram of deterministic bunching and antibunching scattering outcomes is presented with a single energy scale characterizing the increase of the effective barrier height due to interaction of coincident electrons. We suggest clear-cut experimental strategies to detect the predicted effects and give analytical estimates of conditions when the classical dynamics is expected to dominate over quantum effects.

Structural and electronic properties of Weyl semimetal WTe2 under high pressure

The structural and electronic properties of WTe2 are studied from ambient pressure to 30.0 ​GPa. The pressure-induced structural phase transition is found from Td phase to 1T′ phase above 10.0 ​GPa by lattice offset, which is also reflected at approximately 11.2 ​GPa based on the discontinuous electrical parameters. A pair of hole wave and electron wave packets of Td phase gradually overlap revealing the reversible Td-to-1T′ phase structural transition. WTe2 is observed to undergo semimetal-to-semiconductor transition owing to the calculated energy band up to 15 ​GPa, which is also observed at 11.2 ​GPa according to the resistivity-temperature curves under compression and decompression conditions. The electronic density of states at the Fermi level is mainly contributed by the d orbital of W and the p and s orbital of Te. The photoconductivity property is shown by the theoretical and experimental methods.

Potential energy surfaces for electron dynamics from a model of localized Gaussian wave packets with valence-bond spin-coupling: High-harmonic generation spectra from H and He atoms

Potential energy surfaces of electron dynamics (ePES) are constructed from a model of localized electron wave packets (eWP) with non-orthogonal valence-bond (VB) spin coupling and applied to quantum dynamics simulations of high harmonic generation (HHG) spectra of hydrogen and helium atoms induced by intense laser pulses. The dynamics of the single electron on the ePES is calculated by numerically solving the time-dependent Schrödinger equation. The results reasonably reproduce previous studies. The dynamics of the electron wave function, dipole moment and dipole acceleration were analyzed by comparing one- and two-dimensional calculations. It was found that the main part of the wave function remains within a few Bohrs of the nuclear position, while the part of the wave function that is several orders of magnitude smaller in probability density, which escapes the laser-induced potential barrier by quantum tunneling effect, mainly contributes to the HHG.

Energy natural orbital characterization of nonadiabatic electron wavepackets in the densely quasi-degenerate electronic state manifold.

Dynamics and energetic structure of largely fluctuating nonadiabatic electron wavepackets are studied in terms of Energy Natural Orbitals (ENOs) [K. Takatsuka and Y. Arasaki, J. Chem. Phys. 154, 094103 (2021)]. Such huge fluctuating states are sampled from the highly excited states of clusters of 12 boron atoms (B12), which have densely quasi-degenerate electronic excited-state manifold, each adiabatic state of which gets promptly mixed with other states through the frequent and enduring nonadiabatic interactions within the manifold. Yet, the wavepacket states are expected to be of very long lifetimes. This excited-state electronic wavepacket dynamics is extremely interesting but very hard to analyze since they are usually represented in large time-dependent configuration interaction wavefunctions and/or in some other complicated forms. We have found that ENO gives an invariant energy orbital picture to characterize not only the static highly correlated electronic wavefunctions but also those time-dependent electronic wavefunctions. Hence, we first demonstrate how the ENO representation works for some general cases, choosing proton transfer in water dimer and electron-deficient multicenter chemical bonding in diborane in the ground state. We then penetrate with ENO deep into the analysis of the essential nature of nonadiabatic electron wavepacket dynamics in the excited states and show the mechanism of the coexistence of huge electronic fluctuation and rather strong chemical bonds under very random electron flows within the molecule. To quantify the intra-molecular energy flow associated with the huge electronic-state fluctuation, we define and numerically demonstrate what we call the electronic energy flux.

Attosecond streaking of sub-cycle electron wave packets for probing rescattering dynamics in an intense laser field

Attosecond streaking of sub-cycle electron wave packets for probing rescattering dynamics in an intense laser field

Wave-packet propagation in a graphene geometric diode

Dynamics of electron wave-packets is studied using the continuum Dirac model in a graphene geometric diode where the propagation of the wave packet is favored in certain direction due to the presence of geometric constraints. Clear rectification is obtained in the THz frequency range with the maximum rectification level of 3.25, which is in good agreement with recent experiments on graphene ballistic diodes. The rectification levels are considerably higher for systems with narrower channels. In this case, the wave packet transmission probabilities and rectification rate also strongly depend on the energy of the incident wave packet, as a result of the quantum nature of energy levels along such channels. These findings can be useful for fundamental understanding of the charge carrier dynamics in graphene geometry diodes.

Formation of probability and current waves at the scattering of a Gaussian wave packet by a double quantum well

Annotation. A numerical-analytical simulation of scattering by a three-barrier heterostructure of an electronic Gaussian wave packet, the spectral width of which is on the order of the distance between the levels of the doublet of quasi-stationary states, is carried out. This article proves that as a result of scattering, damped waves of electron charge and current densities are formed outside the double well, their characteristics are determined by the structure of the initial wave packet and the poles of the scattering amplitudes. The frequency of these waves is equal to the difference frequency of the doublet, the wavenumber is the difference between the wave numbers of free motion of electrons with resonant energies, and the speed of their propagation is the ratio of these quantities. The system can go into the regime of repetition or amplification of the emission of electron waves if a periodic resonant pumping of the doublet population is provided by scattering of a series of coherent wave packets.

Attosecond Imaging of Electronic Wave Packets.

An electronic wave packet has significant spatial evolution besides its temporal evolution, due to the delocalized nature of composing electronic states. The spatial evolution was not previously accessible to experimental investigations at the attosecond timescale. A phase-resolved two-electron-angular-streaking method is developed to image the shape of the hole density of an ultrafast spin-orbit wave packet in the krypton cation. Furthermore, the motion of an even faster wave packet in the xenon cation is captured for the first time: An electronic hole is refilled 1.2fs after it is produced, and the hole filling is observed on the opposite side where the hole is born.

Charge transport in two-dimensional disordered systems with an external electric field

In this paper, we consider a square lattice with correlated random hopping terms under the effect of an external electric field. We analyzed the dynamics of an initially localized electronic wave packet using a Taylor formalism to solve the Schrödinger dynamic equation. Our calculations suggest that the correlated disorder promotes a fast electronic propagation for intermediate times. When we switch on a static electric field, we observe an oscillatory behavior similar to the well-known “Bloch oscillations” phenomenology. We calculate the frequency of these oscillations, and our results are in good agreement with those predicted by the semi-classical approach used in crystalline lattices. Based on the local disorder and in the absence of extended states in our model, we discussed the stability of these apparent “Bloch oscillations”.

Quantum Interference between Fundamentally Different Processes Is Enabled by Shaped Input Wavefunctions.

This work presents a general framework for quantum interference between processes that can involve different fundamental particles or quasi-particles. This framework shows that shaping input wavefunctions is a versatile and powerful tool for producing and controlling quantum interference between distinguishable pathways, beyond previously explored quantum interference between indistinguishable pathways. Two examples of quantum interference enabled by shaping in interactions between free electrons, bound electrons, and photons are presented: i) the vanishing of the zero-loss peak by destructive quantum interference when a shaped electron wavepacket couples to light, under conditions where the electron's zero-loss peak otherwise dominates; ii) quantum interference between free electron and atomic (bound electron) spontaneous emission processes, which can be significant even when the free electron and atom are far apart, breaking the common notion that a free electron and an atom must be close by to significantly affect each other's processes. Conclusions show that emerging quantum wave-shaping techniques unlock the door to greater versatility in light-matter interactions and other quantum processes ingeneral.