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Register a new userSub-cycle ionization dynamics revealed by trajectory resolved, elliptically-driven high-order harmonic generation
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Esben Witting Larsen
Publication date
2015
fields
Physics
and research's language is
English
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The sub-cycle dynamics of electrons driven by strong laser fields is central to the emerging field of attosecond science. We demonstrate how the dynamics can be probed through high-order harmonic generation, where different trajectories leading to the same harmonic order are initiated at different times, thereby probing different field strengths. We find large differences between the trajectories with respect to both their sensitivity to driving field ellipticity and resonant enhancement. To accurately describe the ellipticity dependence of the long trajectory harmonics we must include a sub-cycle change of the initial velocity distribution of the electron and its excursion time. The resonant enhancement is observed only for the long trajectory contribution of a particular harmonic when a window resonance in argon, which is off-resonant in the field-free case, is shifted into resonance due to a large dynamic Stark shift.
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We study the effect of Coulomb potential on high-order harmonic generation (HHG) numerically and analytically. We focus on the influence of Coulomb potential on emission times of HHG associated with specific electron trajectories. By using a numerical procedure based on numerical solution of time-dependent Schr{o}dinger equation (TDSE) in three dimensions, we extract the HHG emission times both for long and short electron trajectories. We compare TDSE predictions with those of a Coulomb-modified model arising from strong-field approximation (SFA). We show that the Coulomb effect induces earlier HHG emission times than those predicted by the general SFA model without considering the Coulomb potential. In particular, this effect influences differently on long and short electron trajectories and is more remarkable for low-energy harmonics than high ones. It also changes the HHG amplitudes for long and short electron trajectories. We validate our discussions with diverse laser parameters and forms of Coulomb potential. Our results strongly support a four-step model of HHG.
We investigate how short and long electron trajectory contributions to high harmonic emission and their interferences give access to intra-molecular dynamics. In the case of unaligned molecules, we show experimental evidences that the long trajectory signature is more dependent upon the molecule than the short one, providing a high sensitivity to cation nuclear dynamics within 100s of as to few fs. Using theoretical approaches based on Strong Field Approximation and Time Dependent Schrodinger Equation, we examine how quantum path interferences encode electronic motion whilst molecules are aligned. We show that the interferences are dependent on channels superposition and upon which ionisation channel is involved. In particular, quantum path interferences encodes electronic migration signature while coupling between channels is allowed by the laser field. Hence, molecular quantum path interferences is a promising method for Attosecond Spectroscopy, allowing the resolution of ultra-fast charge migration in molecules after ionisation in a self-referenced manner.
We investigate the interwoven dynamic evolutions of neutral nitrogen molecules together with nitrogen ions created through transient tunnel ionization in an intense laser field. By treating the molecules as open quantum systems, it is found that considering real-time injection of ions and strong couplings among their electronic states, nitrogen molecular ions are primarily populated in the electronically excited states, rather than staying in the ground state as predicted by the well-known tunneling theory. The unexpected result is attributed to sub-cycle switch-on of time-dependent polarization by transient ionization and dynamic Stark shift mediated near-resonant multiphoton transitions. Their combined contribution also causes that the vibrational distribution of N$_2^+$ does not comply with Franck-Condon principle. These findings corroborate the mechanism of nitrogen molecular ion lasing and are likely to be universal. The present work opens a new route to explore the important role of transient ionization injection in strong-field induced non-equilibrium dynamics.
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We study high-order harmonic generation (HHG) in model atoms driven by plasmonic-enhanced fields. These fields result from the illumination of plasmonic nanostructures by few-cycle laser pulses. We demonstrate that the spatial inhomogeneous character of the laser electric field, in a form of Gaussian-shaped functions, leads to an unexpected relationship between the HHG cutoff and the laser wavelength. Precise description of the spatial form of the plasmonic-enhanced field allows us to predict this relationship. We combine the numerical solutions of the time-dependent Schrodinger equation (TDSE) with the plasmonic-enhanced electric fields obtained from 3D finite element simulations. We additionally employ classical simulations to supplement the TDSE outcomes and characterize the extended HHG spectra by means of their associated electron trajectories. A proper definition of the spatially inhomogeneous laser electric field is instrumental to accurately describe the underlying physics of HHG driven by plasmonic-enhanced fields. This characterization opens new perspectives for HHG control with various experimental nano-setups
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