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Quantum Effects in Strong Field Physics

Boroumand, Neda

Published Nov 25, 2025• 0 citations
Publisher

Abstract

When matter is exposed to strong fields, electrons are ionized and a number of processes such as high harmonic generation (HHG), above threshold ionization (ATI), non-sequential ionization happen. These processes are usually investigated semiclassically, i.e. matter is treated by quantum mechanics, and radiation is treated classically. In particular HHG which is the generation of ultrashort coherent extreme ultraviolet (XUV) pulses, has enabled a wealth of novel ultrashort spectroscopic methods in atomic, molecular, and condensed matter physics. Further, ionization has applications in micro-machining. Strong field physics continues to have numerous open questions. As an illustration, the mechanisms underlying dominant HHG pathways in solids remain insufficiently understood. It is not clear which mechanism dominates HHG in various materials. Possible pathways are the interband and intraband contributions. Furthermore, many of these processes in strong field physics have been described by single active electron (SAE) approximation. This approach relies on the assumption that the interaction between a single electron and the intense laser field dominates all other interactions. However, this is clearly not the case especially in solids where interactions with the lattice and other electrons can be important. In addition, quantum optical aspects of strong field physics have generated increasing interest, yet they remain partially explored. This chapter involves treating electromagnetic fields using the formalism of second quantization. Quantum optical properties, such as squeezing, entanglement and the negativity of the Wigner function, are of fundamental importance for the field of quantum information and quantum computation. The central theme of my thesis is the development of quantum optical and statistical theoretical frameworks for describing intense laser field processes such as ionization and HHG in atomic and molecular gases and in solids. The second chapter focuses on gaining a detailed understanding of the mathematical steps involved in the Keldysh theory of ionization to establish a solid theoretical foundation. Through this analysis we identified an additional factor of two compared to Keldysh’s original derivation of atomic ionization rates. The third chapter addresses the inadequately understood mechanisms that govern dominant high harmonic generation (HHG) pathways in solids. One approach to clarify these mechanisms involves introducing real (resonant) and virtual processes. We developed the strong field adiabatic following (SFAF) formalism which is based on Dyson expansion using the von-Neumann equation of density matrix. Using SFAF a diagnostic method is obtained to separate virtual and resonant channels. Through this separation, and by comparing with experimental results, we identified the need to incorporate many-body effects. The fourth chapter explores the fact that a solid is a complex many body system in which the SAE approximation is very crude. The electron interacts with holes, other electrons, collective excitations such as plasmons, and phonons. Our work is based on the idea that all theses effects can be treated as a quantum statistical heat bath of bosonic harmonic oscillators. We apply this to our SFAF formalism. In the ionization case, this work has settled a long standing issue which is the fact that simple phenomenological approaches such as the relaxation time approximation 𝑇2 result in nonphysical enhancement of ionization. In chapter five, we have investigated ways to transfer quantum optical properties on the otherwise classical high harmonic radiation. The goal is to use HHG to scale quantum sources to smaller wavelengths. Quantum properties can be imprinted by perturbing HHG with a quantum field, such as bright squeezed vacuum (BSV). In this chapter, the theory of quantum sideband high harmonic generation (QSHHG) in atoms and solids is derived to find ways by which to transfer quantum properties from the perturbative BSV to the harmonic sideband. The theoretical framework is a quantum generalization of the semi-classical Lewenstein model of HHG. It gives closed-form solutions for the HHG and QSHHG wavefunctions. Knowing the wavefunction, we can identify the quantum properties of QSHHG. The additional photons absorbed and emitted from the quantum perturbation, here BSV, create entanglement between individual harmonic sidebands and between the harmonic sidebands and the BSV. We show how this entanglement can be used to create a variety of non-classical states commonly used in quantum information science, such as high-purity single-photon states, Schrödinger cat states, and photon-added squeezed vacuum states. Some of these non-Gaussian states with negative Wigner functions have been shown to provide a quantum computational advantage over their Gaussian counterparts. Additionally, they play a significant role in quantum metrology, enhancing precision measurements beyond classical limits. This chapter has opened a path to quantum engineering of HHG.

DOI
10.20381/ruor-31547

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When matter is exposed to strong fields, electrons are ionized and a number of processes such as high harmonic generation (HHG), above threshold ionization (ATI), non-sequential ionization happen. These processes are usually investigated semiclassically, i.e. matter is treated by quantum mechanics, and radiation is treated classically. In particular HHG which is the generation of ultrashort coherent extreme ultraviolet (XUV) pulses, has enabled a wealth of novel ultrashort spectroscopic methods in atomic, molecular, and condensed matter physics. Further, ionization has applications in micro-machining. Strong field physics continues to have numerous open questions. As an illustration, the mechanisms underlying dominant HHG pathways in solids remain insufficiently understood. It is not clear which mechanism dominates HHG in various materials. Possible pathways are the interband and intraband contributions. Furthermore, many of these processes in strong field physics have been described by single active electron (SAE) approximation. This approach relies on the assumption that the interaction between a single electron and the intense laser field dominates all other interactions. However, this is clearly not the case especially in solids where interactions with the lattice and other electrons can be important. In addition, quantum optical aspects of strong field physics have generated increasing interest, yet they remain partially explored. This chapter involves treating electromagnetic fields using the formalism of second quantization. Quantum optical properties, such as squeezing, entanglement and the negativity of the Wigner function, are of fundamental importance for the field of quantum information and quantum computation. The central theme of my thesis is the development of quantum optical and statistical theoretical frameworks for describing intense laser field processes such as ionization and HHG in atomic and molecular gases and in solids. The second chapter focuses on gaining a detailed understanding of the mathematical steps involved in the Keldysh theory of ionization to establish a solid theoretical foundation. Through this analysis we identified an additional factor of two compared to Keldysh’s original derivation of atomic ionization rates. The third chapter addresses the inadequately understood mechanisms that govern dominant high harmonic generation (HHG) pathways in solids. One approach to clarify these mechanisms involves introducing real (resonant) and virtual processes. We developed the strong field adiabatic following (SFAF) formalism which is based on Dyson expansion using the von-Neumann equation of density matrix. Using SFAF a diagnostic method is obtained to separate virtual and resonant channels. Through this separation, and by comparing with experimental results, we identified the need to incorporate many-body effects. The fourth chapter explores the fact that a solid is a complex many body system in which the SAE approximation is very crude. The electron interacts with holes, other electrons, collective excitations such as plasmons, and phonons. Our work is based on the idea that all theses effects can be treated as a quantum statistical heat bath of bosonic harmonic oscillators. We apply this to our SFAF formalism. In the ionization case, this work has settled a long standing issue which is the fact that simple phenomenological approaches such as the relaxation time approximation 𝑇2 result in nonphysical enhancement of ionization. In chapter five, we have investigated ways to transfer quantum optical properties on the otherwise classical high harmonic radiation. The goal is to use HHG to scale quantum sources to smaller wavelengths. Quantum properties can be imprinted by perturbing HHG with a quantum field, such as bright squeezed vacuum (BSV). In this chapter, the theory of quantum sideband high harmonic generation (QSHHG) in atoms and solids is derived to find ways by which to transfer quantum properties from the perturbative BSV to the harmonic sideband. The theoretical framework is a quantum generalization of the semi-classical Lewenstein model of HHG. It gives closed-form solutions for the HHG and QSHHG wavefunctions. Knowing the wavefunction, we can identify the quantum properties of QSHHG. The additional photons absorbed and emitted from the quantum perturbation, here BSV, create entanglement between individual harmonic sidebands and between the harmonic sidebands and the BSV. We show how this entanglement can be used to create a variety of non-classical states commonly used in quantum information science, such as high-purity single-photon states, Schrödinger cat states, and photon-added squeezed vacuum states. Some of these non-Gaussian states with negative Wigner functions have been shown to provide a quantum computational advantage over their Gaussian counterparts. Additionally, they play a significant role in quantum metrology, enhancing precision measurements beyond classical limits. This chapter has opened a path to quantum engineering of HHG.
The generation of higher-order harmonic radiation originating from the interaction of intense laser pulses with matter is typically described semiclassically: While the electronic structure and dynamics of matter is described quantum mechanically, the intense light field is described classically---and accordingly the generated harmonic radiation. However, pioneering experiments on quantum optical properties of high-order harmonic generation (HHG) in atomic gases from the group of P. Tzallas [I. Gonoskov et al., Sci. Rep. 6, 32821 (2016) and N. Tsatrafyllis et al., Nat. Commun. 8, 15170 (2017)], and theoretical investigations from the group of M. Lewenstein [M. Lewenstein et al., Nat. Phys. 17, 1104 (2021) and P. Stammer et al., Phys. Rev. Lett. 128, 123603 (2022)] have impressively demonstrated that light's quantum properties are observable in the strong-field realm. In this paper, we develop a quantum optical description of HHG in a bulk semiconductor originating from the nonlinear Bloch current. This mechanism of HHG, known as the intraband current, constitutes the major contribution to the emission spectrum for harmonic with energies of quanta roughly below the bandgap. Under certain approximations, employing a quantum description of both light and matter, we obtain analytical solutions, which allow us to analyze the classical and quantum optical characteristics of the fundamental mode of light and the harmonic modes. We find intricate but sufficiently mild modifications of the photon statistics of the fundamental mode and coherent displacements depending on the parameters of the driving laser field. Similar to high-harmonic generation in atoms, the fundamental and emitted harmonic field modes are entangled. Moreover, our analytical model predicts parameter ranges where these quantum optical properties will be most pronounced, allowing protocols for quantum information processing with high photon numbers over a large range of frequencies.
High-order harmonic generation (HHG) is a significant nonlinear phenomenon triggered by the interaction of intense laser fields with matter. As a high-quality coherent light source, it has found extensive applications in areas such as attosecond pulse generation and ultrafast spectroscopy. Recent studies have revealed the prevalent existence of nonclassical effects in high-harmonic radiation, including nonclassical photon statistics, intermodal correlations, and entanglement. It holds broad development prospects in directions including the generation of nonclassical states with high photon numbers, precise control of entanglement in solid-state systems, and integration with cavity quantum electrodynamics. This review systematically summarizes the research progress concerning the nonclassical effects in HHG. It begins with an overview of the semiclassical model and strong-field quantum theory, clarifying the differences in the quantum properties of harmonic fields when driven by coherent states versus nonclassical states. Subsequently, it focuses on various physical schemes for generating nonclassical optical field states, such as optical cat states and squeezed states, via this process. Research on strong-field HHG not only deepens our understanding of the fundamental nature of intense laser physics but also opens new avenues for the generation and application of quantum light sources in the extreme ultraviolet to X-ray spectral regions.
The past thirty years witnessed rapid developing of strong field physics that leads to the first generation of attosecond (10−18 s) pulses. The duration of available pulses has recently been reduced to less than 100 as, approaching the Kepler period of a classical electron revolving around the nucleus. For the first time, electron motions inside atoms, molecules and solids can be traced, probed and even steered in real time. It pushed the study on ultrafast dynamic processes into a new frontier, giving birth to attosecond physics. The development of attosecond pulses provides unprecedented coherent ultrashort XUV (extreme ultra-violet) of soft X-ray sources that enable imaging the atomic structure and resolving the related quantum dynamics for matter science. In particular, it allows the probing and monitoring of electron dynamics in the natural time scale of attoseconds with atomic spatial resolution. The generation and applications of attosecond pulses are directly related to the control and manipulation of the sub-cycle electron dynamics. Recent studies on the correlated multielectron dynamics have provided insight into the optical and dynamical properties of matter in the perspectives of time, phase and entanglement. It deepens our understanding on some of the fundamental questions, e.g., how the single or multiple photons are absorbed and how short are the quantum processes such as photoionization, tunneling ionization and charge migration. Although currently attosecond pulses are limited by the flux and pulse duration, the combination of attosecond pulses with intense infrared laser pulses paves new ways of controlling and probing electron dynamics in the domains of energy, time and space that lays the foundation for petahertz optoelectronics and attosecond pulse based transient spectroscopy. In this review, we will first briefly summarize the advancement of strong field and ultrafast physics including the relevant experimental findings, the theoretical explorations, the related technologies and the possible applications. Then we focus on the sub-cycle electron or multielectron dynamics and their manifestation on the ionization and coherent radiation properties. We start with the time behavior of Fano resonance and how it can be probed in time domain. In section 2, the correlated electron dynamics is discussed in term of anti-screening effect and Pauli effect that influence strong field ionization and high harmonic generation processes. In section 3, the coherent emission with frequency from terahertz to soft XUV and their joint measurement are discussed by emphasizing the generation mechanism of terahertz wave in two-color laser pulses. The developed high-harmonic and terahertz wave spectroscopy (HATS) is shown capable of imaging the molecular structure and dynamics. In section 4, the time-resolving of electron and hole dynamics and their coherence is proposed based on attosecond transient absorption technique. The coherence of ionization and the correlated electron dynamics is hinted crucial for electron-hole interaction. The topics are very limited and mainly selected from the perspectives of our group.
High-order harmonic generation is a highly nonlinear phenomenon in which ultraviolet photons are generated when an atom is subjected to a high-intensity infrared laser field. This process has been extensively studied, but most of the formulations employ a semiclassical approach in which the electron is treated quantum mechanically while the driving field is treated classically. Although some recent studies follow a quantum-optical approach, the existing descriptions do not offer much insight into the physical processes taking place, and are always limited to monochromatic driving fields. In this thesis, we construct a fully quantized framework for strong-field ionization and high-harmonic generation that allows for quantization of both the driving field and the ultraviolet emission. The presented formalism extends the Strong-Field Approximation theory to a quantum-optical framework, with which we can obtain an analytical expression for the electron and the driving field after the interaction.
We analytically describe the strong-field light-electron interaction using a quantized coherent laser state with arbitrary photon number. We obtain a light-electron wave function which is a closed-form solution of the time-dependent Schrödinger equation (TDSE). This wave function provides information about the quantum optical features of the interaction not accessible by semi-classical theories. With this approach we can reveal the quantum optical properties of high harmonic generation (HHG) process in gases by measuring the photon statistics of the transmitted infrared (IR) laser radiation. This work can lead to novel experiments in high-resolution spectroscopy in extreme-ultraviolet (XUV) and attosecond science without the need to measure the XUV light, while it can pave the way for the development of intense non-classical light sources.
Recent developments in quantum light engineering have enabled the use of infrared bright squeezed vacuum (BSV) femtosecond pulses in nonlinear optics, including strong-field physics and high-harmonic generation. However, theory has focused on single-atom interactions, neglecting the crucial macroscopic aspect of light propagation through media. This raises a key question: How does BSV propagate in nonlinear media, and how this affects the nonlinear signals and the radiation’s quantumness? We address this with a fully quantized framework for propagation in gas media undergoing high-harmonic generation. We find that ionization and the associated photon losses cause decoherence, which limits the propagation length, degrades radiation’s quantumness, and reduces the emitted harmonics. However, these effects are not detrimental. We identify conditions that minimize propagation-induced decoherence while preserving detectable harmonics with super-Poissonian photon statistics. Our results establish fully quantized basis for exploring BSV in nonlinear optics, strong-field-quantum optics, and ultrafast science in all states of matter. Recent developments in strong-field quantum optics are usually modelled with approaches neglecting the propagation dynamics inside the medium. Here, the authors introduce a fully quantized framework for bright squeezed vacuum states propagating inside atomic media undergoing high-harmonic generation, unveiling the role of decoherence effects.