Local excitation and valley polarization in graphene with multi-harmonic pulses.

We elucidate the mechanism of strong laser pulse excitation in pristine graphene with multi-harmonic pulses, linearly polarized parallel to the line connecting the two different Dirac points in the Brillouin zone and with a maximal vector potential given by the distance of those points. The latter two conditions have emerged from our previous work [Kelardeh et al., Phys. Rev. Res., 2022, 4, L022014] as favorable for large valley polarization. We introduce a novel compacted representation for excitation, locally resolved in the initial conditions for the crystal momenta. These maps are our main tool to gain insight into the excitation dynamics. They also help with understanding the effect of dephasing. We work out why a long wavelength and a moderate number of overtones in the harmonic pulse generate the largest valley polarizations.

Perspectives for analyzing non-linear photo-ionization spectra with deep neural networks trained with synthetic Hamilton matrices.

We have constructed deep neural networks, which can map fluctuating photo-electron spectra obtained from noisy pulses to spectra from noise-free pulses. The network is trained on spectra from noisy pulses in combination with random Hamilton matrices, representing systems which could exist but do not necessarily exist. In [Giri et al., Phys. Rev. Lett., 2020, 124, 113201] we performed a purification of fluctuating spectra, that is, mapping them to those from Fourier-limited Gaussian pulses. Here, we investigate the performance of such neural-network-based maps for predicting spectra of double pulses, pulses with a chirp and even partially-coherent pulses from fluctuating spectra generated by noisy pulses. Secondly, we demonstrate that along with purification of a fluctuating double-pulse spectrum, one can estimate the time-delay of the underlying double pulse, an attractive feature for single-shot spectra from SASE FELs. We demonstrate our approach with resonant two-photon ionization, a non-linear process, sensitive to details of the laser pulse.

Proper Time Delays Measured by Optical Streaking.

In attosecond science it is assumed that Wigner-Smith time delays, known from scattering theory, are determined by measuring streaking shifts. Despite their wide use from atoms to solids this has never been proven. Analyzing the underlying process-energy absorption from the streaking light-we derive this relation. It reveals that only under specific conditions streaking shifts measure Wigner-Smith time delays. For the most relevant case, interactions containing long-range Coulomb tails, we show that finite streaking shifts, including relative shifts from two different orbitals, are misleading. We devise a new time-delay definition and describe a measurement technique that avoids the record of a complete streaking scan, as suggested by the relation between time delays and streaking shifts.

Purifying Electron Spectra from Noisy Pulses with Machine Learning Using Synthetic Hamilton Matrices.

Photoelectron spectra obtained with intense pulses generated by free-electron lasers through self-amplified spontaneous emission are intrinsically noisy and vary from shot to shot. We extract the purified spectrum, corresponding to a Fourier-limited pulse, with the help of a deep neural network. It is trained on a huge number of spectra, which was made possible by an extremely efficient propagation of the Schrödinger equation with synthetic Hamilton matrices and random realizations of fluctuating pulses. We show that the trained network is sufficiently generic such that it can purify atomic or molecular spectra, dominated by resonant two- or three-photon ionization, nonlinear processes which are particularly sensitive to pulse fluctuations. This is possible without training on those systems.

Universal High-Energy Photoelectron Emission from Nanoclusters Beyond the Atomic Limit.

Rescattering by electrons on classical trajectories is central to understand photoelectron and high-harmonic emission from isolated atoms or molecules in intense laser pulses. By controlling the cluster size and the quiver amplitude of electrons, we demonstrate how rescattering influences the energy distribution of photoelectrons emitted from noble gas nanoclusters. Our experiments reveal a universal dependence of photoelectron energy distributions on the cluster size when scaled by the field driven electron excursion, establishing a unified rescattering picture for extended systems with the known atomic dynamics as the limit of zero extension. The result is supported by molecular dynamics calculations and rationalized with a one-dimensional classical model.

Adiabatic Passage to the Continuum: Controlling Ionization with Chirped Laser Pulses.

We demonstrate that, by changing the direction of the chirp in vacuum-ultraviolet pulses, one can switch between excitation and ionization with very high contrast, if the carrier frequency of the light is resonant with two bound states. This is a surprising consequence of rapid adiabatic passage if extended to include transitions to the continuum. The chirp phase locks the linear combination of the two resonantly coupled bound states whose ionization amplitudes interfere constructively or destructively depending on the chirp direction under suitable conditions. We derive the phenomenon in a minimal model and verify the effect with calculations for helium as a realistic example.

Electron Dynamics Driven by Light-Pulse Derivatives.

We demonstrate that ultrashort pulses carry the possibility for a new regime of light-matter interaction with nonadiabatic electron processes sensitive to the envelope derivative of the light pulse. A standard single pulse with its two peaks in the derivative separated by the width of the pulse acts in this regime like a traditional double pulse. The two ensuing nonadiabatic ionization bursts have slightly different ionization amplitudes. This difference is due to the redistribution of continuum electron energy during the bursts, negligible in standard photoionization. A time-dependent close-coupling approach based on cycle-averaged potentials in the Kramers-Henneberger reference frame permits a detailed understanding of light-pulse derivative-driven electron dynamics.

Essential Conditions for Dynamic Interference.

We develop general quantitative criteria for dynamic interference, a manifestation of a double-slit interference in time which should be realizable with brilliant state-of-the-art high-frequency laser sources. Our analysis reveals that the observation of dynamic interference hinges upon maximizing the difference between the dynamic polarization of the initial bound and the final continuum states of the electron during the light pulse while keeping depletion of the initial state small. These two properties, Stark shift and depletion, can be determined from electronic structure calculations avoiding expensive propagation in time. Confirmed by numerical results, we predict that this is impossible for the hydrogen ground state but feasible for excited states; this has been exemplified for the case of the hydrogen 2p state.

Enhancing scattering images for orientation recovery with diffusion map.

We explore the possibility for orientation recovery in single-molecule coherent diffractive imaging with diffusion map. This algorithm approximates the Laplace-Beltrami operator, which we diagonalize with a metric that corresponds to the mapping of Euler angles onto scattering images. While suitable for images of objects with specific properties we show why this approach fails for realistic molecules. We introduce a modification of the form factor in the scattering images which facilitates the orientation recovery and should be suitable for all recovery algorithms based on the distance of individual images.

Tunneling Ionization Time Resolved by Backpropagation.

We determine the ionization time in tunneling ionization by an elliptically polarized light pulse relative to its maximum. This is achieved by a full quantum propagation of the electron wave function forward in time, followed by a classical backpropagation to identify tunneling parameters, in particular, the fraction of electrons that has tunneled out. We find that the ionization time is close to zero for single active electrons in helium and in hydrogen if the fraction of tunneled electrons is large. We expect our analysis to be essential to quantify ionization times for correlated electron motion.

Dynamical Characteristics of Rydberg Electrons Released by a Weak Electric Field.

The dynamics of ultraslow electrons in the combined potential of an ionic core and a static electric field is discussed. With state-of-the-art detection it is possible to create such electrons through strong intense-field photoabsorption and to detect them via high-resolution time-of-flight spectroscopy despite their very low kinetic energy. The characteristic feature of their momentum spectrum, which emerges at the same position for different laser orientations, is derived and could be revealed experimentally with an energy resolution of the order of 1 meV.

Prevailing features of x-ray-induced molecular electron spectra revealed with fullerenes.

X-ray photoabsorption from intense short pulses by a molecule triggers complicated electron and subsequently ion dynamics, leading to photoelectron spectra, which are difficult to interpret. Illuminating fullerenes offers a way to separate out the electron dynamics since the cage structure confines spatially the origin of photo- and Auger electrons. Together with the sequential nature of the photoprocesses at intensities available at x-ray free-electron lasers, this allows for a remarkably detailed interpretation of the photoelectron spectra, as we will demonstrate. The general features derived can serve as a paradigm for less well-defined situations in other large molecules or clusters.

Spatial correlations in finite samples revealed by Coulomb explosion.

We demonstrate that fast removal of many electrons uncovers initial correlations of atoms in a finite sample through a pronounced peak in the kinetic-energy spectrum of the exploding ions. This maximum is the result of an intricate interplay between the composition of the system from discrete particles and its boundary. The formation of the peak can be described analytically, accounting for correlations beyond a mean-field reference model. It can be experimentally detected with short and intense light pulses from 4th-generation light sources.

Proton ejection from molecular hydride clusters exposed to strong x-ray pulses.

Clusters consisting of small molecules containing hydrogen do eject fast protons when illuminated by short x-ray pulses. A suitable overall charging of the cluster controlled by the x-ray intensity induces electron migration from the surface to the bulk leading to efficient segregation of the protons and to a globally hindered explosion of the heavy atoms even outside the screened volume. We investigate this peculiar effect systematically along the isoelectronic sequence of methane over ammonia and water to the atomic limit of neon as a reference. In contrast to core-shell systems where the outer shell is sacrificed to reduce radiation damage, the intricate proton dynamics of hydride clusters allows one to keep the entire backbone of heavy atoms intact.

Electron-energy bunching in laser-driven soft recollisions.

We introduce soft recollisions in laser-matter interaction. They are characterized by the electron missing the ion upon recollision in contrast with the well-known head-on collisions responsible for high-harmonic generation or above-threshold ionization. We demonstrate analytically that soft recollisions can cause a bunching of photoelectron energies through which a series of low-energy peaks emerges in the electron yield along the laser polarization axis. This peak sequence is universal, it does not depend on the binding potential, and is found below an excess energy of one tenth of the ponderomotive energy.

Massively parallel ionization of extended atomic systems.

Massively parallel ionization of many atoms in a cluster or biomolecule is identified as a new phenomenon of light-matter interaction which becomes feasible through short and intense FEL pulses. Almost simultaneously emitted from the illuminated target the photo-electrons can have such a high density that they interact substantially even after photoionization. This interaction results in a characteristic electron spectrum which can be interpreted as a convolution of a mean-field electron dynamics and binary electron-electron collisions. We demonstrate that this universal spectrum can be obtained analytically by summing synthetic two-body Coulomb collision events. Moreover, we propose an experiment with hydrogen clusters to observe massively parallel ionization.

Monitoring atomic cluster expansion by high-harmonic generation.

High-harmonic generation is shown to be capable of providing time-resolved information about the particle density of a complex system. As an example, we study numerically high-harmonic generation from expanding xenon clusters in a pump-probe laser scheme, where the pump laser pulse induces the cluster explosion and the probe pulse generates harmonics in the expanding cluster. We show that the high-harmonic spectra characterize the properties of the expanding cluster. Hence, measuring the dependence of the harmonic signal on the pump-probe delay suggests itself as an experimental tool to monitor many-particle dynamics with unique temporal resolution; based on optical measurements, this technique is naturally free from any spatial charge effects.

Suppression of exponential electronic decay in a charged environment.

Inner-shell ionization of atoms and molecules leads to the creation of highly excited ionic states that often decay by electron emission. The dynamics of the decay is usually assumed to be exponential and the process is characterized by a decay rate. Here we show that in a multiply ionized cluster created by interaction with a high-intensity free-electron laser (FEL) radiation, trapping of the emitted electron by the neighboring ions changes the character of the decay dynamics qualitatively to the extent that it can become oscillatory instead of exponential. Implications of the predicted effect on Coster-Kronig and interatomic Coulombic decay processes induced by FELs are investigated.

Laser-driven nanoplasmas in doped helium droplets: local ignition and anisotropic growth.

Doping a helium nanodroplet with only a tiny xenon cluster of a few atoms sparks complete ionization of the droplet at laser intensities below the ionization threshold of helium atoms. As a result, the intrinsically inert and transparent droplet turns into a fast and strong absorber of infrared light. Microscopic calculations reveal a two-step mechanism to be responsible for the dramatic change: Avalanchelike ionization of the helium atoms on a femtosecond time scale, driven by field ionization due to the quickly charged xenon core, is followed by resonant absorption enabled by an unusual cigar-shaped nanoplasma within the droplet.

Rescattering for extended atomic systems.

Laser-driven rescattering of electrons is the basis of many strong-field phenomena in atoms and molecules. Here, we will show how this mechanism operates in extended atomic systems, giving rise to effective energy absorption. Rescattering from extended systems can also lead to energy loss, which in its extreme form results in nonlinear light-induced trapping. Intense-laser interaction with atomic clusters is discussed as an example. We explain fast electron emission, seen in experimental and numerically obtained spectra, by rescattering of electrons at the highly charged cluster.