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Optics and Spectroscopy

Control for atom response in multicomponent laser fields

A. V. Andreev, Sergey Yu Stremoukhov, Olga A. Shoutova

Published Mar 1, 2012• 1 citation
Publisher

Abstract

A theory of the nonlinear optical response of an atom interacting with a superposition of arbitrarily polarized fields is developed. The theory is based on the analytical solution of the boundary-value problem for an electron moving in a spherically symmetric intraatomic field and in the field of an external electromagnetic field. By means of the example of an argon atom interacting with a bichromatic field formed by the first and second harmonics of a Ti:sapphire laser, it is shown that, when an atom interacts with the field of two polarized pulses the polarization directions of which are not collinear, the response spectrum significantly depends on the laser radiation parameters—the duration and intensity of pulses, the time of delay between them, and the angle between the directions of polarization vectors. Generation of THz radiation is shown to be possible in the ionization-free regime due to intraatomic nonlinearity.

DOI
10.1134/s0030400x12030022

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A theory of the nonlinear optical response of an atom interacting with a superposition of arbitrarily polarized fields is developed. The theory is based on the analytical solution of the boundary-value problem for an electron moving in a spherically symmetric intraatomic field and in the field of an external electromagnetic field. By means of the example of an argon atom interacting with a bichromatic field formed by the first and second harmonics of a Ti:sapphire laser, it is shown that, when an atom interacts with the field of two polarized pulses the polarization directions of which are not collinear, the response spectrum significantly depends on the laser radiation parameters—the duration and intensity of pulses, the time of delay between them, and the angle between the directions of polarization vectors. Generation of THz radiation is shown to be possible in the ionization-free regime due to intraatomic nonlinearity.
Polarization response that appears in silver vapors in the field of a high-intensity femtosecond Ti:sapphire laser has been studied by the direct numerical integration of the time-dependent Schrödinger equation. The regions of applicability have been determined for perturbation theory and the power series expansion of the polarization in the field. The contribution of free electrons to the response at the frequency of the interacting field has been calculated, which is due to the photoionization process and limits the Kerr effect. An important contribution of laser-excited atomic states to nonlinear atomic responses of neutral atoms has been demonstrated.
The interaction of intense laser fields with matter is accompanied by a multitude of phenomena, ranging from the generation of coherent radiation across various spectral ranges (from terahertz to soft X-rays) to the creation of beams of accelerated charged particles and micromodification of the volume and surface of various samples.To describe this diversity of phenomena, several theoretical approaches have been developed to date.These approaches utilize different approximations to address this complex nonlinear problem, allowing for the explanation of specific aspects of such interactions.The developed theoretical frameworks consider the interaction at both microscopic and macroscopic levels; at the microscopic level, they investigate the characteristics of single atoms interacting with laser fields, while at the macroscopic level, they analyze nonlinear susceptibilities that describe the nonlinear polarization of the medium during the propagation of laser radiation through it.This work presents an overview of methods describing some of the most commonly employed theoretical approaches to model the response of a medium at a microscopic (quantum-mechanical) level, as well as various methods for controlling the properties of generated coherent radiation.A model for the gas medium is described that accounts for both the response characteristics of individual atoms and allows for consideration of phase and quasiphase matching effects during radiation generation.The influence of medium parameters on the efficiency of generation and polarization properties of generated radiation is analyzed under both phase and quasi-phase matching conditions.A detailed description of an analytical method for calculating the nonlinear susceptibility of a gas medium is provided.The obtained values of nonlinear susceptibility for arbitrary orders may be useful in numerical calculations concerning the propagation of laser radiation in matter.Various channels for radiation generation are analyzed as parameters of the laser field are varied.
The theory of the interaction of a centrosymmetric atom with a superstrong spatially inhomogeneous laser field is developed. This theory employs the two-level approximation to describe the dynamics of spatially nonlocal interactions related to variations in the populations of the levels. We propose a model that includes spatially nonlocal interactions, such as magnetic-dipole and quadrupole interactions and interactions due to the gradient of the ponderomotive potential of the field. We consider the interaction of a homogeneous medium of centrosymmetric atoms with a superstrong laser field, which is represented as a superposition of two plane-wave ultrashort pulses propagating at some angle with respect to each other. Perturbation theory, which is valid for the fields of moderate intensity, is developed for the atomic response. The results of numerical simulations are compared with the predictions of this perturbation theory. The specific features of the nonlinear-optical response of an atom in a superstrong field are investigated. The angular distribution of the second- and third-harmonic emission is calculated in the constant-field approximation for different polarisations of the incident field.
A novel kind of coherent control of various atomic and molecular photoprocesses proceeding in a bichromatic electromagnetic (EM) laser field, angular coherent control , is proposed and demonstrated here theoretically by studying the particular case of negative-ion photodetachment in the field of a linearly polarized fundamental laser frequency and its second harmonic of arbitrary spatial configuration and orientation of the unit polarization vectors e 1 and e 2 of the respective harmonic fields. Due to the inherent spatial asymmetry of the applied bichromatic field, the ejection of detached photoelectrons is also generally asymmetric in respect of the detached photoelectron momentum replacement p →- p . As follows from our gauge-invariant analytical calculations within the framework of perturbation theory on EM interaction and a zero-range potential model for the negative ion, this field asymmetry results in a photocurrent, the magnitude and direction of which are strongly dependent on both the relative phase shift Φ between the harmonics of the ionizing bichromatic field and on the angle θ between the polarization vectors e 1 and e 2 . The latter strong dependence on the angle θ is the background for angular control of the direction and magnitude of the produced photocurrent by means of an appropriate choice and proper adjustment of the angle between the polarization vectors of the incident bichromatic field harmonics.