arXiv subjects

Serguei Patchkovskii

Publications and source records attributed to Serguei Patchkovskii.

44 records · Page 3Linked to original sources

arXiv2018

Control of attosecond light polarization in two-color bi-circular fields

We develop theoretically and confirm both numerically and experimentally a comprehensive analytical model which describes the propensity rules in the emission of circularly polarized high harmonics by systems driven by two-color counter-rotating fields, a fundamental and its second harmonic. We identify and confirm the three propensity rules responsible for the contrast between the 3N+1 and 3N+2 harmonic lines in the HHG spectra of noble gas atoms. We demonstrate how these rules depend on the laser parameters and how they can be used in the experiment to shape the polarization properties of the emitted attosecond pulses.

physics.atom-ph↗

arXiv2018

Strong-field control and enhancement of chiral response in bi-elliptical high-order harmonic generation: an analytical model

The generation of high-order harmonics in a medium of chiral molecules driven by intense bi-elliptical laser fields can lead to strong chiroptical response in a broad range of harmonic numbers and ellipticities [D. Ayuso et al, J. Phys. B 51, 06LT01 (2018)]. Here we present a comprehensive analytical model that can describe the most relevant features arising in the high-order harmonic spectra of chiral molecules driven by strong bi-elliptical fields. Our model recovers the physical picture underlying chiral high-order harmonic generation based on ultrafast chiral hole motion and identifies the rotationally invariant molecular pseudoscalars responsible for chiral dynamics. Using the chiral molecule propylene oxide as an example, we show that one can control and enhance the chiral response in bi-elliptical high-order harmonic generation by tailoring the driving field, in particular by tuning its frequency, intensity and ellipticity, exploiting a suppression mechanism of achiral background based on the linear Stark effect.

physics.optics↗

arXiv2017

Full-dimensional treatment of short-time vibronic dynamics in molecular high-harmonics generation process in methane

We present derivation and implementation of the Multi-Configurational Strong-Field Approximation with Gaussian nuclear Wave Packets (MC-SFA-GWP) -- a version of the molecular strong-field approximation which treats all electronic and nuclear degrees of freedom, including their correlations, quantum-mechanically. The technique allows, for the first time, realistic simulation of high-harmonic emission in polyatomic molecules without invoking reduced-dimensionality models for the nuclear motion or the electronic structure. We use MC-SFA-GWP to model isotope effects in high-harmonics generation (HHG) spectroscopy of methane. The HHG emission in this molecule transiently involves strongly vibronically-coupled $^2F_2$ electronic state of the $\rm CH_4^+$ cation. We show that the isotopic HHG ratio in methane contains signatures of: a) field-free vibronic dynamics at the conical intersection (CI); b) resonant features in the recombination cross-sections; c) laser-driven bound-state dynamics; as well as d) the well-known short-time Gaussian decay of the emission. We assign the intrinsic vibronic feature (a) to a relatively long-lived ($\ge4$ fs) vibronic wave packet of the singly-excited $ν_4$ ($t_2$) and $ν_2$ ($e$) vibrational modes, strongly coupled to the components of the $^2F_2$ electronic state. We demonstrate that these physical effects differ in their dependence on the wavelength, intensity, and duration of the driving pulse, allowing them to be disentangled. We thus show that HHG spectroscopy provides a versatile tool for exploring both conical intersections and resonant features in photorecombination matrix elements in the regime not easily accessible with other techniques.

physics.chem-ph↗

arXiv2016

Strong-field ionization of clusters using two-cycle pulses at 1.8~$μ$m

The interaction of intense laser pulses with nano-scale particles leads to the production of high-energy electrons, ions, neutral atoms, neutrons and photons. Up to now, investigations have focused on near-infrared to X-ray laser pulses consisting of many optical cycles. Here we study strong-field ionization of rare-gas clusters ($10^3$ to $10^5$ atoms) using two-cycle 1.8~$μ$m laser pulses to access a new interaction regime in the limit where the electron dynamics are dominated by the laser field and the cluster atoms do not have time to move significantly. The emission of fast electrons with kinetic energies exceeding 3keV is observed using laser pulses with a wavelength of 1.8~$μ$m and an intensity of $1\times 10^{15}$~W/cm$^2$, whereas only electrons below 500eV are observed at 800nm using a similar intensity and pulse duration. Fast electrons are preferentially emitted along the laser polarization direction, showing that they are driven out from the cluster by the laser field. In addition to direct electron emission, an electron rescattering plateau is observed. Scaling to even longer wavelengths is expected to result in a highly directional current of energetic electrons on a few-femtosecond timescale.

physics.atm-clus↗

arXiv2015

Opportunities for chiral discrimination using high harmonic generation in tailored laser fields

Chiral discrimination with high harmonic generation (cHHG method) has been introduced in the recent work by R. Cireasa et al ( Nat. Phys. 11, 654 - 658, 2015). In its original implementation, the cHHG method works by detecting high harmonic emission from randomly oriented ensemble of chiral molecules driven by elliptically polarized field, as a function of ellipticity. Here we discuss future perspectives in the development of this novel method, the ways of increasing chiral dichroism using tailored laser pulses, new detection schemes involving high harmonic phase measurements, and concentration-independent approaches. Using the example of the epoxypropane molecule C$_3$H$_6$O (also known as 1,2-propylene oxide), we show theoretically that application of two-color counter-rotating elliptically polarized laser fields yields an order of magnitude enhancement of chiral dichroism compared to single color elliptical fields. We also describe how one can introduce a new functionality to cHHG: concentration-independent measurement of the enatiomeric excess in a mixture of randomly oriented left-handed and right-handed molecules. Finally, for arbitrary configurations of laser fields, we connect the observables of the cHHG method to the amplitude and phase of chiral response, providing a basis for reconstructing wide range of chiral dynamics from cHHG measurements, with femtosecond to sub-femtosecond temporal resolution.

physics.optics↗

arXiv2013

Grand-Canonical Quantized Liquid Density-Functional Theory in a Car-Parrinello Implementation

Quantized Liquid Density-Functional Theory [Phys. Rev. E 2009, 80, 031603], a method developed to assess the adsorption of gas molecules in porous nanomaterials, is reformulated within the grand canonical ensemble. With the grand potential it is possible to compare directly external and internal thermodynamic quantities. In our new implementation, the grand potential is minimized utilizing the Car-Parrinello approach and gives, in particular for low temperature simulations, a significant computational advantage over the original canonical approaches. The method is validated against original QLDFT, and applied to model potentials and graphite slit pores.

cond-mat.mtrl-sci↗

arXiv2012

Mechanisms of two-color laser-induced field-free molecular orientation

Two mechanisms of two-color (ω+ 2ω) laser-induced field-free molecular orientation, based on the hyperpolarizability and ionization depletion, are explored and compared. The CO molecule is used as a computational example. While the hyperpolarizability mechanism generates small amounts of orientation at intensities below the ionization threshold, ionization depletion quickly becomes the dominant mechanism as soon as ionizing intensities are reached. Only the ionization mechanism leads to substantial orientation (e.g. on the order of | | > 0.1). For intensities typical of laser-induced molecular alignment and orientation experiments, the two mechanism lead to robust, characteristic timings of the field-free orientation wave-packet revivals relative to the the alignment revivals and the revival time. The revival timings can be used to detect the active orientation mechanism experimentally.

physics.atom-ph↗

arXiv2009

One-Electron Ionization of Multielectron Systems in Strong Nonresonant Laser Fields

We present a novel approach to calculating strong field ionization dynamics of multielectron molecular targets. Adopting a multielectron wavefunction ansatz based on field-free ab initio neutral and ionic multielectron states, a set of coupled time-dependent single-particle Schroedinger equations describing the neutral amplitude and continuum electron are constructed. These equations, amenable to direct numerical solution or further analytical treatment, allow one to study multielectron effects during strong field ionization, recollision, and high harmonic generation. We apply the method to strong field ionization of CO_2, and suggest the importance of intermediate core excitation to explain previous failure of analytical models to reproduce experimental ionization yields for this molecule.

physics.atom-ph↗