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Physical Review A

Nonlinear optical response of noble gases via the metastable electronic state approach

Anand Bahl, Ewan M. Wright, M. Kolesík

Published Aug 29, 2016• 12 citations
Publisher

Abstract

The goal of this paper is to elucidate the theoretical underpinnings of the metastable electronic state approach (MESA) and demonstrate its utility for the evaluation of the nonlinear optical response of noble-gas atoms with emphasis on the application of the method to the propagation of multicolor optical fields in large-scale, spatially resolved simulations. More specifically, single-active-electron models of various atoms are employed to calculate their nonlinear properties both within the adiabatic approximation, involving a single metastable state and beyond, capturing inertial effects, and wavelength-dependent ionization. Simulations for excitation pulses at different center wavelengths as well as ionization in two-color pulses are presented and compared with numerical solutions of the time-dependent Schr\"odinger equation. Illustrative examples of the numerical simulation of high-power pulse propagation incorporating MESA data are also presented and showcase the successful application to optical filamentation in the midinfrared region.

DOI
10.1103/physreva.94.023850

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The goal of this paper is to elucidate the theoretical underpinnings of the metastable electronic state approach (MESA) and demonstrate its utility for the evaluation of the nonlinear optical response of noble-gas atoms with emphasis on the application of the method to the propagation of multicolor optical fields in large-scale, spatially resolved simulations. More specifically, single-active-electron models of various atoms are employed to calculate their nonlinear properties both within the adiabatic approximation, involving a single metastable state and beyond, capturing inertial effects, and wavelength-dependent ionization. Simulations for excitation pulses at different center wavelengths as well as ionization in two-color pulses are presented and compared with numerical solutions of the time-dependent Schr"odinger equation. Illustrative examples of the numerical simulation of high-power pulse propagation incorporating MESA data are also presented and showcase the successful application to optical filamentation in the midinfrared region.
We present a simple model for the nonlinear optical response of atomic gases for pulses with center wavelengths in the transparency region and peak fields for which ionization is not prevalent. By comparing with simulations based on the Schrödinger equation for a hydrogen atom we demonstrate that the model accurately captures the dispersion of the nonlinear polarization as well as noninstantaneous effects for a variety of photon energies and also a two-color pulse. Our approach should be of utility in simulating near- and mid-infrared pulse propagation in dielectric media for which extreme nonlinear effects can arise.
This dissertation demonstrates the usefulness of exactly solvable quantum models in the investigation of light-matter interaction phenomena associated with the propagation of ultrashort laser pulses through gaseous media. This work fits into the larger research effort towards remedying the weaker portions of the standard set of medium modeling equations commonly used in simulations. The ultimate goal is to provide a self-consistent quantum mechanical description that can integrate Maxwell and Schrödinger systems and provide a means to realistically simulate nonlinear optical experiments on relevant scales. The study of exactly solvable models begins with one of the simplest quantum systems available, one with a 1D Dirac-delta function potential plus interaction with the light field. This model contains, in the simplest form, the most important "ingredients" that control optical filamentation, i.e. discrete and continuum electronic states. The importance of both states is emphasized in the optical intensity regime in which filaments form, where both kinds of electronic states simultaneously play a role and may not even be distinguishable. For this model atom, an analytical solution for the time-dependent light-induced atomic response from an arbitrary excitation waveform is obtained. Although this system is well-known and has been studied for decades, this result is probably the most practically useful and general one obtained thus far. Numerical implementation details of the result are also given as the task is far from trivial. Given an efficient implementation, the model is used in light-matter interaction simulations and from these it is apparent that even this toy model can qualitatively reproduce many of the nonlinear phenomena seen in experiments. Not only does this model capture the basic physics of optical filamentation, but it is also well-suited for high harmonic generation simulations. Next, a theoretical framework for using Stark resonant states (or metastable states) to represent the medium's polarization response is presented. Researchers have recognized long ago the utility of Gamow resonant states as a description of various decay processes. Even though a bound electron experiences a similar decay-like process as it transitions into the continuum upon ionization, it was unclear whether field-induced Stark resonant states carry physically relevant information. It is found that they do, and in particular it is possible to use them to capture a medium's polarization response. To this end, two quantum systems with potentials represented by a 1D Dirac-delta function and a 1D square well are solved, and all the necessary quantities for their use as medium models are presented. From these results it is possible to conjecture some general properties that hold for all resonance systems, including systems that reside in higher than one dimensional space. Finally, as a practical application of this theory, the Metastable Electronic State Approach (MESA) is presented as a quantum-based replacement for the standard medium modeling equations.
We investigate the propagation of ultrashort laser pulses in atomic rubidium vapor. The pulses are intensive enough to ionize the atoms and are directly resonant with the 780-nm D2{D}_{2}D2​ line. We derive a relatively simple theory for computing the nonlinear optical response of atoms and investigate the competing effects of strong resonant nonlinearity and ionization in the medium using computer simulations. A nonlinear self-channeling of pulse energy is found to produce a continuous plasma channel with complete ionization. We evaluate the length, width, and homogeneity of the resulting plasma channel for various values of pulse energy and initial focusing to identify regimes optimal for applications in plasma-wave accelerator devices such as that being built by the AWAKE collaboration at CERN. Similarities and differences with laser pulse filamentation in atmospheric gases are discussed.
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.
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.