Attosecond delays in X-ray molecular ionization.

The photoelectric effect is not truly instantaneous but exhibits attosecond delays that can reveal complex molecular dynamics1-7. Sub-femtosecond-duration light pulses provide the requisite tools to resolve the dynamics of photoionization8-12. Accordingly, the past decade has produced a large volume of work on photoionization delays following single-photon absorption of an extreme ultraviolet 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. Here we report measurements of the X-ray photoemission delay of core-level electrons, with unexpectedly large delays, ranging up to 700 as in NO near the oxygen K-shell threshold. These measurements exploit attosecond soft X-ray pulses from a free-electron laser to scan across the entire region near the K-shell threshold. Furthermore, we find that the delay spectrum is richly modulated, suggesting several contributions, including transient trapping of the photoelectron owing 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.

Symphony on strong field approximation.

This paper has been prepared by the Symphony collaboration (University of Warsaw, Uniwersytet Jagiellonski, 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 (HHG), above-threshold ionization (ATI), and non-sequential multielectron ionization (NSMI). 'Simple man's models' provide both an intuitive basis for understanding the numerical solutions of the time-dependent Schrödinger 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 the SFA is a method to solve the TDSE, in which the non-perturbative interactions are described by including continuum-continuum interactions in a systematic perturbation-like theory. In this review we focus on recent applications of the SFA to HHG, ATI and NSMI from multi-electron atoms and from multi-atom molecules. The main novel part of the presented theory concerns generalizations of the SFA to: (i) time-dependent treatment of two-electron atoms, allowing for studies of an interplay between electron impact ionization and resonant excitation with subsequent ionization; (ii) time-dependent treatment in the single active electron approximation of 'large' molecules and targets which are themselves undergoing dynamics during the HHG or ATI processes. 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. We dedicate this work to the memory of Bertrand Carré, who passed away in March 2018 at the age of 60.

Tunneling Time and Weak Measurement in Strong Field Ionization.

Tunneling delays represent a hotly debated topic, with many conflicting definitions and little consensus on when and if such definitions accurately describe the physical observables. Here, we relate these different definitions to distinct experimental observables in strong field ionization, finding that two definitions, Larmor time and Bohmian time, are compatible with the attoclock observable and the resonance lifetime of a bound state, respectively. Both of these definitions are closely connected to the theory of weak measurement, with Larmor time being the weak measurement value of tunneling time and Bohmian trajectory corresponding to the average particle trajectory, which has been recently reconstructed using weak measurement in a two-slit experiment [S. Kocsis, B. Braverman, S. Ravets, M. J. Stevens, R. P. Mirin, L. K. Shalm, and A. M. Steinberg, Science 332, 1170 (2011)]. We demonstrate a big discrepancy in strong field ionization between the Bohmian and weak measurement values of tunneling time, and we suggest this arises because the tunneling time is calculated for a small probability postselected ensemble of electrons. Our results have important implications for the interpretation of experiments in attosecond science, suggesting that tunneling is unlikely to be an instantaneous process.

High-order harmonic generation from a thin film crystal perturbed by a quasi-static terahertz field.

Studies of laser-driven strong field processes subjected to a (quasi-)static field have been mainly confined to theory. Here we provide an experimental realization by introducing a bichromatic approach for high harmonic generation (HHG) in a dielectric that combines an intense 70 femtosecond duration mid-infrared driving field with a weak 2 picosecond period terahertz (THz) dressing field. We address the physics underlying the THz field induced static symmetry breaking and its consequences on the efficient production/suppression of even-/odd-order harmonics, and demonstrate the ability to probe the HHG dynamics via the modulation of the harmonic distribution. Moreover, we report a delay-dependent even-order harmonic frequency shift that is proportional to the time derivative of the THz field. This suggests a limitation of the static symmetry breaking interpretation and implies that the resultant attosecond bursts are aperiodic, thus providing a frequency domain probe of attosecond transients while opening opportunities in precise attosecond pulse shaping.

Extraction of higher-order nonlinear electronic response in solids using high harmonic generation.

Nonlinear susceptibilities are key to ultrafast lightwave driven optoelectronics, allowing petahertz scaling manipulation of the signal. Recent experiments 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. The highly nonlinear nature of high harmonic generation (HHG) has the potential to extract even higher order nonlinear susceptibility terms. 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. Our results open a door to multi-channel signal processing, controlled by laser polarization.

Complete chaotic synchronization in mutually coupled time-delay systems.

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 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 subsystems.

Predictions of ultraharmonic oscillations in coupled arrays of limit cycle oscillators.

Coupled distinct arrays of nonlinear oscillators have been shown to have a regime of high frequency, or ultraharmonic, 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 antiphase state. The underlying mechanism for the creation and stability of the ultraharmonic oscillations is analyzed. A class of interarray 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.

Temporally-coherent terawatt attosecond XFEL synchronized with a few cycle laser.

Attosecond metrology using laser-based high-order harmonics has been significantly advanced and applied to various studies of electron dynamics in atoms, molecules and solids. Laser-based high-order harmonics have a limitation of low power and photon energies. There is, however, a great demand for even higher power and photon energy. Here, we propose a scheme for a terawatt attosecond (TW-as) X-ray pulse in X-ray free-electron laser controlled by a few cycle IR pulse, where one dominant current spike in an electron bunch is used repeatedly to amplify a seeded radiation to a terawatt level. This scheme is relatively simple, compact, straightforward, and also produces a temporally and spectrally clean pulse. The viability of this scheme is demonstrated in simulations using Pohang accelerator laboratory (PAL)-XFEL beam parameters.

Control of traveling-wave oscillations and bifurcation behavior in central pattern generators.

Understanding synchronous and traveling-wave oscillations, particularly as they relate to transitions between different types of behavior, is a central problem in modeling biological systems. Here, we address this problem in the context of central pattern generators (CPGs). We use contraction theory to establish the global stability of a traveling-wave or synchronous oscillation, determined by the type of coupling. This opens the door to better design of coupling architectures to create the desired type of stable oscillations. We then use coupling that is both amplitude and phase dependent to create either globally stable synchronous or traveling-wave solutions. Using the CPG motor neuron network of a leech as an example, we show that while both traveling and synchronous oscillations can be achieved by several types of coupling, the transition between different types of behavior is dictated by a specific coupling architecture. In particular, it is only the "repulsive" but not the commonly used phase or rotational coupling that can explain the transition to high-frequency synchronous oscillations that have been observed in the heartbeat pattern generator of a leech. This shows that the overall dynamics of a CPG can be highly sensitive to the type of coupling used, even for coupling architectures that are widely believed to produce the same qualitative behavior.

Disease extinction in the presence of random vaccination.

We investigate disease extinction in an epidemic model described by a birth-death process. We show that, in the absence of vaccination, 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 random vaccination leads to an exponential increase in the extinction rate, with the exponent that strongly depends on the vaccination parameters.

Synchronized dynamics of cortical neurons with time-delay feedback.

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 pre-synaptic input during the inter-spike 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.