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The photoelectric effect is not truly instantaneous, but exhibits attosecond delays that can reveal complex molecular dynamics. Sub-femtosecond duration light pulses provide the requisite tools to resolve the dynamics of photoionization. Accordingly, the past decade has produced a large volume of work on photoionization delays following single photon absorption of an extreme ultraviolet (XUV) photon. However, the measurement of time-resolved core-level photoionization remained out of reach. The required x-ray photon energies needed for core-level photoionization were not available with attosecond tabletop sources. We have now measured the x-ray photoemission delay of core-level electrons, and here report unexpectedly large delays, ranging up to 700 attoseconds in NO near the oxygen K-shell threshold. These measurements exploit attosecond soft x-ray pulses from a free-electron laser (XFEL) to scan across the entire region near the K-shell threshold. Furthermore, we find the delay spectrum is richly modulated, suggesting several contributions including transient trapping of the photoelectron due to shape resonances, collisions with the Auger-Meitner electron that is emitted in the rapid non-radiative relaxation of the molecule, and multi-electron scattering effects. The results demonstrate how x-ray attosecond experiments, supported by comprehensive theoretical modelling, can unravel the complex correlated dynamics of core-level photoionization.

The nearly free electron metal next to a localized Mott insulating state has been recently proposed as a way to probe Kondo lattice physics and to gain insight into how the two extremes of localized and delocalized electron states interact (Sunko, et al, Science advances 6, 2020). Although high harmonic generation has been used extensively to investigate the gas phase, its extension to solids is relatively recent, and has not yet been applied to interfaces. Here, we investigate the field-induced dielectric break-down at the Mott-insulator/metal interface using high harmonic generation, emitted when the interface is subjected to an ultrafast laser pulse. We show that the intensity of high harmonic emission correlates closely with doublon production and the corresponding loss of short-range anti-ferromagnetic order. For strong interlayer coupling, the harmonic intensity is defined by a phase transition between states that do not exist in a pure Mott insulator case. For weak interlayer coupling, the threshold for dielectric breakdown is considerably lowered due to the presence of a metallic layer. This suggests that interlayer coupling can be used as an additional knob to control magnetic insulator break-down, with implications for using Mott insulators as memristors in neuromorphic circuits.

High Harmonic Generation (HHG), which has been widely used in atomic gas, has recently expanded to solids as a means to study highly nonlinear electronic response in condensed matter and produce coherent high frequency radiation with new properties. Most recently, attention has turned to Topological Materials (TMs) and the use of HHG to characterize topological bands and invariants. Theoretical interpretation of nonlinear electronic response in TMs, however, presents many challenges. In particular, the Bloch wavefunction phase of TMs has undefined points in the Brillouin Zone. This leads to singularities in calculating the inter-band and intra-band transition dipole matrix elements of Semiconductor Bloch Equations (SBEs). Here, we use the laser-electromagnetic velocity gauge ${\boldsymbol p}\cdot {\bf A}(t)$ to numerically integrate the SBEs and treat the singularity in the production of the electrical currents and HHG spectra. We use a prototype of Chern Insulators (CIs), the Haldane model, to demonstrate our approach. We find good qualitative agreement of the velocity gauge compared to the length gauge and the Time-Dependent Density Functional theory in the case of topologically trivial materials such as MoS$_2$. For velocity gauge and length gauge, our two-band Haldane model reproduces key HHG spectra features: ($\textit i$) The selection rules for linear and circular light drivers, ($\textit ii$) The linear cut-off law scaling and ($\textit iii$) The anomalous circular dichroism. We conclude that the velocity-gauge approach captures experimental observations and provides theoretical tools to investigate topological materials.

We present a theory of Mott memristors whose working principle is the non-linear carrier avalanche multiplication in Mott insulators subject to strong electric fields. The internal state of the memristor, which determines its resistance, is encoded in the density of doublon and hole excitations in the Mott insulator. In the current-voltage characteristic, insulating and conducting states are separated by a negative-differential-resistance region, leading to hysteretic behavior. Under oscillating voltage, the response of a voltage-controlled, non-polar memristive system is obtained, with retarded current and pinched hysteresis loop. As a first step towards neuromorphic applications, we demonstrate self-sustained spiking oscillations in a circuit with a parallel capacitor. Being based on electronic excitations only, this memristor is up to several orders of magnitude faster than previous proposals relying on Joule heating or ionic drift., Comment: 13 pages, 10 figures

In this report, a novel methodology based on the static coherent states approach is introduced with the capability of calculating various strong-field laser-induced nonlinearities in full dimensional single-electron molecular systems; an emphasis is made on the high-order harmonic generation. To evaluate the functionality of this approach, we present a case study of the Hydrogen molecular ion \ih interacting with a few-cycle linearly polarized optical laser with trapezoidal waveform. We detected that the accuracy of the obtained harmonics is considerably enhanced by averaging the expectation value of the acceleration of the single electron over a set of identical random simulations. Subsequently, the presented approach demands a significantly lower number of basis sets than the regular exact three dimensional unitary split-operator solvers of time dependent Schr{\"o}dinger equation that necessitate an extremely large number of data points in the coordinate space, and so the computational cost. Additionally, applying static coherent states method, we have investigated isolated attosecond pulse generation using the polarization gating technique, which combines two delayed counter rotating circular laser pulses, and opens up a gate at the central portion of the superposed pulse., Comment: 9 pages, 6 figures

State-of-the-art experiments employ strong ultrafast optical fields to study the nonlinear response of electrons in solids on an attosecond time-scale. Notably, a recent experiment retrieved a 3rd order nonlinear susceptibility by comparing the nonlinear response induced by a strong laser field to a linear response induced by the otherwise identical weak field. In parallel, experiments have demonstrated high harmonic generation (HHG) in solids, a highly nonlinear process that until recently had only been observed in gases. The highly nonlinear nature of HHG has the potential to extract even higher order nonlinear susceptibility terms, and thereby characterize the entire response of the electronic system to strong field excitation. However, up till now, such characterization has been elusive due to a lack of direct correspondence between high harmonics and nonlinear susceptibilities. Here, we demonstrate a regime where such correspondence can be clearly made, extracting nonlinear susceptibilities (7th, 9th, and 11th) from sapphire of the same order as the measured high harmonics. The extracted high order susceptibilities show angular-resolved periodicities arising from variation in the band structure with crystal orientation. Nonlinear susceptibilities are key to ultrafast lightwave driven optoelectronics, allowing petahertz scaling manipulation of the signal. Our results open a door to multi-channel signal processing, controlled by laser polarization.

This paper has been prepared by the Symphony collaboration (University of Warsaw, Uniwersytet Jagiello\'nski, DESY/CNR and ICFO) on the occasion of the 25th anniversary of the "simple man's models" which underlie most of the phenomena that occur when intense ultrashort laser pulses interact with matter. The phenomena in question include High-Harmonic Generation, Above-Threshold Ionization, and Non-Sequential Multielectron Ionization. "Simple man's models" provide, both an intuitive basis for understanding the numerical solutions of the time-dependent Schr\"odinger equation, and the motivation for the powerful analytic approximations generally known as the Strong Field Approximation (SFA). In this paper we first review the SFA in the form developed by us in the last 25 years. In this approach SFA is a method to solve the TDSE using a systematic perturbation theory in a part of the Hamiltonian describing continuum-continuum transitions in the presence of the laser field. In this review we focus on recent applications of SFA to HHG, ATI and NSMI from multi-electron atoms and from multi-atom. The main novel part of the presented theory concerns generalizations of SFA to: (i) time-dependent treatment of two-electron atoms, allowing for studies of an interplay between Electron Impact Ionization (EII) and Resonant Excitation with Subsequent Ionization (RESI); (ii) time-dependent treatment in the single active electron (SAE) approximation of "large" molecules and targets which are themselves undergoing dynamics during the HHG or ATI process. In particular, we formulate the general expressions for the case of arbitrary molecules, combining input from quantum chemistry and quantum dynamics. We formulate also theory of time-dependent separable molecular potentials to model analytically the dynamics of realistic electronic wave packets for molecules in strong laser fields., Comment: We dedicate this work to the memory of Bertrand Carr\'e, who passed away in March 2018 at the age of 60. This Accepted Manuscript is available under the CC BY-NC-ND license (https://creativecommons.org/licenses/by-nc-nd/3.0/)

The use of semiclassical models based on the Strong Field Approximation (SFA) is ubiquitous in strong field multi-photon ionization and underlies many key developments in attosecond science, including the description of High Harmonic Generation (HHG). However, such models are notably lacking in streaking experiments, which use an attosecond pulse to initiate single-photon ionization and a lower frequency infrared pulse to provide timing information. Here, we introduce a classical Wigner propagation (CWP) method, which analogously to semiclassical models in strong field ionization, treats the ionization step quantum mechanically, followed subsequently by classical propagation (with initial conditions obtained from the Wigner function) in the infrared probe field. As we demonstrate, this method compares well with experimental data and full two-electron quantum simulations available for helium, includes multi-electron effects, and can be applied to molecules, where the full solution of the time-dependent Schrodinger equation is not feasible. Applying the CWP method to a many-atom molecule, like 2,3,3-trimethyl-butyl-2-iodide, we find a relatively significant directional dependence of streaking delays, indicating the importance of orientation-resolved measurements in molecules.

Emission of high-order harmonics from solids provides a new avenue in attosecond science. On one hand, it allows to investigate fundamental processes of the non-linear response of electrons driven by a strong laser pulse in a periodic crystal lattice. On the other hand, it opens new paths toward efficient attosecond pulse generation, novel imaging of electronic wave functions, and enhancement of high-order harmonic generation (HHG) intensity. A key feature of HHG in a solid (as compared to the well-understood phenomena of HHG in an atomic gas) is the delocalization of the process, whereby an electron ionized from one site in the periodic lattice may recombine with any other. Here, we develop an analytic model, based on the localized Wannier wave functions in the valence band and delocalized Bloch functions in the conduction band. This Wannier-Bloch approach assesses the contributions of individual lattice sites to the HHG process, and hence addresses precisely the question of localization of harmonic emission in solids. We apply this model to investigate HHG in a ZnO crystal for two different orientations, corresponding to wider and narrower valence and conduction bands, respectively. Interestingly, for narrower bands, the HHG process shows significant localization, similar to harmonic generation in atoms. For all cases, the delocalized contributions to HHG emission are highest near the band-gap energy. Our results pave the way to controlling localized contributions to HHG in a solid crystal, with hard to overestimate implications for the emerging area of atto-nanoscience.

By measuring energy spectra of the electron emission from a sharp tungsten tip induced by few-cycle laser pulses, the laser-field dependence of the emission mechanism was investigated. In strong laser fields, we confirm the appearance of laser-driven tunneling emission and find that it can be disentangled from the concomitant photo-excited electron emission, both temporally and spectrally, by the opening of a peculiar emission channel. This channel involves prompt laser-driven tunneling emission and subsequent laser-driven electron re-scattering off the surface, delayed by the electrons traveling far inside the metal before scattering. The quantitative understanding of these processes gives insights on attosecond tunneling emission from solids and should prove useful in designing new types of pulsed electron sources., Comment: 4 pages, 3 figures, submitted to Physical Review Letters

We introduce a method to investigate the longitudinal momentum spread resulting from strong-field tunnel ionization of Helium which, unlike other methods, is valid for all ellipticities of laser pulse. Semiclassical models consisting of tunnel ionization followed by classical propagation in the combined ion and laser field reproduce the experimental results if an initial longitudinal spread at the tunnel exit is included. The values for this spread are found to be of the order of twice the transverse momentum spread.

We compare the main competing theories of tunneling time against experimental measurements using the attoclock in strong laser field ionization of helium atoms. Refined attoclock measurements reveal a real and not instantaneous tunneling delay time over a large intensity regime, using two different experimental apparatus. Only two of the theoretical predictions are compatible within our experimental error: the Larmor time, and the probability distribution of tunneling times constructed using a Feynman Path Integral (FPI) formulation. The latter better matches the observed qualitative change in tunneling time over a wide intensity range, and predicts a broad tunneling time distribution with a long tail. The implication of such a probability distribution of tunneling times, as opposed to a distinct tunneling time, challenges how valence electron dynamics are currently reconstructed in attosecond science. It means that one must account for a significant uncertainty as to when the hole dynamics begin to evolve., Comment: 11 pages, 4 figures

It is well-known from numerical and experimental results that the fraction of Rydberg states (excited neutral atoms) created by tunnel ionization declines dramatically with increasing ellipticity of laser light. We present a method to analyze this dependence on ellipticity, deriving a probability distribution of Rydberg states that agrees closely with recent experimental [1] and numerical results. In particular, contradicting the existing proposed mechanism [1] and general expectations, our results indicate that the dependence of Rydberg yield on laser ellipticity is not caused by a rescattering process. Rather, we show that most Rydberg electrons never come back to the vicinity of the exit point after ionization, and end up relatively far from the atom (compared to the exit point) after the laser pulse has passed. We also present experimental data revealing a bifurcation that corresponds to a cut-off in Rydberg generation, and present an analytic derivation with a perturbative inclusion of the Coloumb force. [1] T. Nubbemeyer, K. Gorling, A. Saenz, U. Eichmann, and W. Sandner, Phys. Rev. Lett. 101, 233001 (2008).

We present an ellipticity resolved study of momentum distributions arising from strong-field ionization of Helium at constant intensity. The influence of the ion potential on the departing electron is considered within a semi-classical model consisting of an initial tunneling step and subsequent classical propagation. We find that the momentum distribution can be explained by the presence of a longitudinal momentum spread of the electron at the exit from the tunnel. Our combined experimental and theoretical study provides an estimate of this momentum spread.

We investigate stochastic extinction in an epidemic model and the impact of random vaccinations in large populations. We show that, in the absence of vaccinations, the effective entropic barrier for extinction displays scaling with the distance to the bifurcation point, with an unusual critical exponent. Even a comparatively weak Poisson-distributed vaccination leads to an exponential increase in the extinction rate, with the exponent that strongly depends on the vaccination parameters., Comment: Accepted for publication to PRL

We consider a line of three mutually coupled lasers with time delays and study chaotic synchronization of the outer lasers. Two different systems are presented: optoelectronically coupled semiconductor lasers and optically coupled fiber lasers. While the dynamics of the two systems are very different, robust synchronization of end lasers is obtained in both cases over a range of parameters. Here, we present analysis and numerical simulation to explain some of the observed synchronization phenomena. First, we introduce the system of three coupled semiconductor lasers and discuss the onset of oscillations that occurs via a bifurcation as the coupling strength increases. Next, we analyze the synchronization of the end lasers by examining the dynamics transverse to synchronized state. We prove that chaotic synchronization of the outer semiconductor lasers will occur for sufficiently long delays, and we make a comparison to generalized synchronization in driven dissipative systems. It is shown that the stability of synchronous state (as indicated by negative Lyupunov exponents transverse to the synchronization manifold) depends on the internal dissipation of the outer lasers. We next present numerical simulations for three coupled fiber lasers, highlighting some of the differences between the semiconductor and fiber laser systems. Due to the large number of coupled modes in fiber lasers, this is a good system for investigating spatio-temporal chaos. Stochastic noise is included in the fiber laser model, and synchrony of the outer lasers is observed even at very small coupling strengths., Comment: 35 pages, 12 figures. to appear in a special review book on "Recent Advances in Nonlinear Laser Dynamics: Control and Synchronization", Research Signpost

We investigate stochastic extinction in an epidemic model and the impact of random vaccinations in large populations formulated in terms of an optimal escape path. We find that different random vaccination strategies can have widely different results in decreasing expected time till extinction, for the same total amount of vaccines used. Vaccination strategies are considered in terms of two parameters: average frequency of vaccinations, given by $\gamma$, and the amplitude of the vaccinations, $\epsilon$, where $\epsilon \ll 1$ refers to the proportion of the population being vaccinated at some particular instant. It is found that while the average number of individuals vaccinated per unit time, $\gamma \epsilon$, is kept constant, the particular values of $\gamma$ and $\epsilon$ can play a highly significant role in increasing the chance of epidemic extinction. The findings suggest that expected time till extinction can be significantly shortened if less frequent vaccinations occur in larger groups, corresponding to low $\gamma$, high $\epsilon$ strategy., Comment: 5 pages, 1 figure

The dynamics of three mutually coupled cortical neurons with time delays in the coupling are explored numerically and analytically. The neurons are coupled in a line, with the middle neuron sending a somewhat stronger projection to the outer neurons than the feedback it receives, to model for instance the relay of a signal from primary to higher cortical areas. For a given coupling architecture, the delays introduce correlations in the time series at the time-scale of the delay. It was found that the middle neuron leads the outer ones by the delay time, while the outer neurons are synchronized with zero lag times. Synchronization is found to be highly dependent on the synaptic time constant, with faster synapses increasing both the degree of synchronization and the firing rate. Analysis shows that presynaptic input during the interspike interval stabilizes the synchronous state, even for arbitrarily weak coupling, and independent of the initial phase. The finding may be of significance to synchronization of large groups of cells in the cortex that are spatially distanced from each other., Comment: 21 pages, 11 figures

Complete chaotic synchronization of end lasers has been observed in a line of mutually coupled, time-delayed system of three lasers, with no direct communication between the end lasers. The present paper uses ideas from generalized synchronization to explain the complete synchronization in the presence of long coupling delays, applied to a model of mutually coupled semiconductor lasers in a line. These ideas significantly simplify the analysis by casting the stability in terms of the local dynamics of each laser. The variational equations near the synchronization manifold are analyzed, and used to derive the synchronization condition that is a function of the parameters. The results explain and predict the dependence of synchronization on various parameters, such as time-delays, strength of coupling and dissipation. The ideas can be applied to understand complete synchronization in other chaotic systems with coupling delays and no direct communication between synchronized sub-systems., Comment: 22 pages, 6 figures

Coupled distinct arrays of nonlinear oscillators have been shown to have a regime of high frequency, or ultra-harmonic, oscillations that are at multiples of the natural frequency of individual oscillators. The coupled array architectures generate an in-phase high-frequency state by coupling with an array in an anti-phase state. The underlying mechanism for the creation and stability of the ultra-harmonic oscillations is analyzed. A class of inter-array coupling is shown to create a stable, in-phase oscillation having frequency that increases linearly with the number of oscillators, but with an amplitude that stays fairly constant. The analysis of the theory is illustrated by numerical simulation of coupled arrays of Stuart-Landau limit cycle oscillators., Comment: 24 pages, 9 figures, accepted to Phys. Rev. E, in press