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Exactly Solvable Light-Matter Interaction Models for Studying Filamentation Dynamics

Jeffrey M. Brown

Published Jan 1, 2016• 0 citations
OpenAlex

Abstract

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.

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In a realistic treatment of a three-dimensional nonlinear optical experiment, the complete Maxwell equations in (3 + 1) space-time dimensions should be employed. It is then necessary to utilize a multi-mode Hamiltonian that correctly describes the propagating modes. There is an important difference between these experiments and traditional particle scattering. Quantum field dynamics in nonlinear media is dominated by multiple scattering, which is the reason why perturbation theory is less useful. Nevertheless, it is interesting to make a link to conventional perturbation theory. Accordingly, we start by considering a perturbative theory of propagation in a one-dimensional nonlinear optical system in a χ (3) medium. While this calculation cannot treat long interaction times, it does give a qualitative understanding of the important features. This problem is the ‘hydrogen atom’ of quantum field theory: it has fully interacting fields with exact solutions for their energy levels. This is because a photon in a waveguide is an elementary boson in one dimension. The interactions between these bosons are mediated by the Kerr effect, which in quantum field theory is a quartic potential, equivalent to a delta-function interaction. The quantum field theory involved is the simplest model of a quantum field that has an exact solution. This elementary model is still nontrivial in terms of its dynamics, as the calculation of quantum dynamics using standard eigenfunction techniques would require exponentially complex sums over multi-dimensional overlap integrals. This is not practicable, and accordingly we use other methods including quantum phase-space representations to solve this problem.

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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.

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The quantum optical description of high-order harmonic generation where both the electrons of the generating medium and the driving and generated light fields are described quantum mechanically has been of significant interest in the past years. The quantum optical formulation leads to equations of motion for the generated light field in which the quantum optical field couples to the time-dependent current of the electronic medium irrespectively of the specifics of the electronic system being an atom, molecule, or solid. These equations of motion are not solvable for any realistic system and accurate and verified approximations are hence needed. In this paper, we present a hierarchy of approximations for the equations of motion for the photonic state. At each level in this hierarchy, we compare it to the previous level justifying the validity using the Fermi-Hubbard model as an example of an electronic system with correlations. This model allows us to perform an accurate simulation of the electron motion of all the required states. We find that for the typical experimental situation of weak quantized-light-matter-coupling constant and at intensities well below the damage threshold, an explicit expression for the generated quantum light, referred to as the Markov-state approximation, captures the high-harmonic spectrum quantitatively and describes the single-mode quantum properties of the generated light as characterized by the Mandel-$Q$ parameter and the degree of squeezing qualitatively.

arXiv:2410.19533•Physical Review A•Jan 22, 2025•11 citations
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.
In a realistic treatment of a three-dimensional nonlinear optical experiment, the complete Maxwell equations in (3 + 1) space-time dimensions should be employed. It is then necessary to utilize a multi-mode Hamiltonian that correctly describes the propagating modes. There is an important difference between these experiments and traditional particle scattering. Quantum field dynamics in nonlinear media is dominated by multiple scattering, which is the reason why perturbation theory is less useful. Nevertheless, it is interesting to make a link to conventional perturbation theory. Accordingly, we start by considering a perturbative theory of propagation in a one-dimensional nonlinear optical system in a χ (3) medium. While this calculation cannot treat long interaction times, it does give a qualitative understanding of the important features. This problem is the ‘hydrogen atom’ of quantum field theory: it has fully interacting fields with exact solutions for their energy levels. This is because a photon in a waveguide is an elementary boson in one dimension. The interactions between these bosons are mediated by the Kerr effect, which in quantum field theory is a quartic potential, equivalent to a delta-function interaction. The quantum field theory involved is the simplest model of a quantum field that has an exact solution. This elementary model is still nontrivial in terms of its dynamics, as the calculation of quantum dynamics using standard eigenfunction techniques would require exponentially complex sums over multi-dimensional overlap integrals. This is not practicable, and accordingly we use other methods including quantum phase-space representations to solve this problem.
Studying how light interacts with materials has become important for many technological applications from optical communication to developing of new materials. Therefore scientists have always tried to improve their understanding of these effects. The primary goal has always been to microscopically describe the pertinent processes. This paper provides a brief introduction into the interactions of atoms with laser fields. Precisely this interaction, photoelectric effect and the blackbody radiation were those findings which started off the development of quantum mechanics. This theory allowed better description of atoms and it will be used in this work to handle the problem we are confronting. We will consider two of the simplest potentials and let the atom interact with a strong laser pulse in these potentials. From this interaction the so called resonant states will arise. The goal of this thesis is to investigate to what extent and in what meaning these resonant states form a complete set of functions and consequently can be used for expansion of atomic states of physical importance.
Until recently, the nonlinear interaction between light and matter has been restricted to only low photon energies produced by optical lasers. However, about a decade ago, the rise of free-electron laser facilities revolutionized the field of nonlinear light-matter interaction by delivering intense high-energy light pulses. Today, such lasers are used for research in materials science, chemical technology, biophysical science, solid state physics as well as fundamental research. It is the new experimental possibilities provided by free-electron lasers that motivated the work presented in this thesis. Two-photon ionization process is one of the simplest nonlinear interactions in which absorption of two photons by an atom (or a molecule) leads to promoting one of its bound electrons to continuum. This work presents studies of two-photon ionization of neutral atoms. After a brief historical introduction to the topic of nonlinear light-matter interaction, the density matrix describing the state of an atom and a photoelectron following two-photon ionization is derived. In each successive chapter, part of this density matrix is used to obtain characteristic quantities such as total two-photon ionization cross section, photoelectron angular distributions, ion polarization or degree of polarization of fluorescence photon produced by subsequent decay of the photoion. Physical properties of these quantities are studied and intriguing phenomena, such as elliptical dichroism, polarization transfer as well as relativistic and screening effects are investigated.
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.
For decades, ultrafast light-matter interactions have provided a powerful means to observe electrons in motion across a wide range of physical systems. This dissertation builds new theoretical frameworks to make sense of the emergent phenomena that arise when light drives matter into the strong-field regime, spanning atomic, molecular, and condensed-matter systems. The resulting dynamics leave their fingerprints on a variety of observables, such as photoionization spectra, high-harmonic generation, and nonlinear spectroscopic signals, each of which provides a different window onto the underlying electronic motion. The work is organized into two parts.The first part focuses on the electric-field observables of nonlinear optical signals. Because both the amplitude and phase of the emitted field are experimentally accessible through techniques such as spectral interferometry and electro-optic sampling, the full field itself serves as a rich observable for characterizing nonlinear responses in atomic, molecular, and condensed-matter systems. Leveraging this, the simulations presented here uncover novel and largely unexplored physical phenomena encoded in these field observables. The second part turns to optical spectroscopy with quantum light. Although nonlinear optical processes are conventionally modeled within a semiclassical framework, treating the matter quantum mechanically while the driving ultrafast fields remain classical, the resulting signals can nonetheless exhibit intrinsically non-classical properties. Building on this insight, a framework for interpreting experimental data is introduced and used to show that four-wave mixing driven by ultrafast femtosecond laser pulses generates bright squeezed light. Beyond squeezed light, strong field-matter interactions can also produce attosecond entangled photons, a distinct form of quantum light. Several strategies are proposed to enhance the efficiency of their generation, with the developed theory predicting rates of energy-time entangled biphoton production orders of magnitude beyond those achievable with conventional spontaneous parametric down-conversion (SPDC) sources. The studies presented here are initial steps toward investigating quantum properties of these systems through quantum phynonlinear spectroscopy, which is not achievable with classical light.
The quantum optical description of high-order harmonic generation where both the electrons of the generating medium and the driving and generated light fields are described quantum mechanically has been of significant interest in the past years. The quantum optical formulation leads to equations of motion for the generated light field in which the quantum optical field couples to the time-dependent current of the electronic medium irrespectively of the specifics of the electronic system being an atom, molecule, or solid. These equations of motion are not solvable for any realistic system and accurate and verified approximations are hence needed. In this paper, we present a hierarchy of approximations for the equations of motion for the photonic state. At each level in this hierarchy, we compare it to the previous level justifying the validity using the Fermi-Hubbard model as an example of an electronic system with correlations. This model allows us to perform an accurate simulation of the electron motion of all the required states. We find that for the typical experimental situation of weak quantized-light-matter-coupling constant and at intensities well below the damage threshold, an explicit expression for the generated quantum light, referred to as the Markov-state approximation, captures the high-harmonic spectrum quantitatively and describes the single-mode quantum properties of the generated light as characterized by the Mandel-QQQ parameter and the degree of squeezing qualitatively.