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Register a new userDetailed study of quantum path interferences in high harmonic generation driven by chirped laser pulses
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Added by
Tam\\'as Csizmadia PhD
Publication date
2021
fields
Physics
and research's language is
English
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We investigate the electron quantum path interference effects during high harmonic generation in atomic gas medium driven by ultrashort chirped laser pulses. To achieve that, we identify and vary the different experimentally relevant control parameters of such a driving laser pulse influencing the high harmonic spectra. Specifically, the impact of the pulse duration, peak intensity and instantaneous frequency is studied in a self-consistent manner based on Lewenstein formalism. Simulations involving macroscopic propagation effects are also considered. The study aims to reveal the microscopic background behind a variety of interference patterns capturing important information both about the fundamental laser field and the generation process itself. The results provide guidance towards experiments with chirp control as a tool to unravel, explain and utilize the rich and complex interplay between quantum path interferences including the tuning of the periodicity of the intensity dependent oscillation of the harmonic signal, and the curvature of spectrally resolved Maker fringes.
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Electron quantum path interferences in strongly laser-driven aligned molecules and their dependence on the molecular alignment is an essential open problem in strong-field molecular physics. Here, we demonstrate an approach which provides direct access to the observation of these interference processes. The approach is based on the combination of the time-gated-ion-microscopy technique with a pump-probe arrangement used to align the molecules and generate high-order harmonics. By spatially resolving the interference pattern produced by the spatiotemporal overlap of the harmonics emitted by the short and long electron quantum paths, we have succeeded in measuring in situ their phase difference and disclose their dependence on molecular alignment. The findings constitute a vital step towards an understanding of strong-field molecular physics and the development of attosecond spectroscopy approaches without the use of auxiliary atomic references.
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 show that high-order harmonics generated from molecules by intense laser pulses can be expressed as the product of a returning electron wave packet and the photo-recombination cross section (PRCS) where the electron wave packet can be obtained from simple strong-field approximation (SFA) or from a companion atomic target. Using these wave packets but replacing the PRCS obtained from SFA or from the atomic target by the accurate PRCS from molecules, the resulting HHG spectra are shown to agree well with the benchmark results from direct numerical solution of the time-dependent Schrodinger equation, for the case of H$_2^+$ in laser fields. The result illustrates that these powerful theoretical tools can be used for obtaining high-order harmonic spectra from molecules. More importantly, the results imply that the PRCS extracted from laser-induced HHG spectra can be used for time-resolved dynamic chemical imaging of transient molecules with temporal resolutions down to a few femtoseconds.
We investigate the polarization properties of high harmonics generated with the bichromatic counterrotating circularly polarized (BCCP) laser fields by numerically solving time-dependent Schrodinger equation (TDSE). It is found that, the helicity of the elliptically polarized harmonic emission is reversed at particular harmonic orders. Based on the time-frequency analysis and the classical three-step model, the correspondence between the positions of helicity
We measure spectrally and spatially resolved high-order harmonics generated in argon using chirped multi-cycle laser pulses. Using a stable, high-repetition rate laser we observe detailed interference structures in the far-field. The structures are of two kinds; off-axis interference from the long trajectory only and on-axis interference including the short and long trajectories. The former is readily visible in the far-field spectrum, modulating both the spectral and spatial profile. To access the latter, we vary the chirp of the fundamental, imparting different phases on the different trajectories, thereby changing their relative phase. Using this method together with an analytical model, we are able to explain the on-axis behaviour and access the dipole phase parameters for the short ((alpha_s)) and long ((alpha_l)) trajectories. The extracted results compare very well with phase parameters calculated by solving the time-dependent Schrodinger equation. Going beyond the analytical model, we are also able to successfully reproduce the off-axis interference structure.
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