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IEEE Lasers and Electro-Optics Society Annual Meeting (LEOS)

The scaling of an intense field nonlinear interaction

Louis F. DiMauro

Published Nov 21, 2003• 0 citations
Publisher

Abstract

In this talk, we will discuss the physics of an alkali metal atom interacting with an intense mid-infrared (3-4 /spl mu/m) laser field. In a Keldysh picture this scaled interaction should show similar ionization dynamics to the more familiar situation of a near visible light interacting with inert gas atoms. However, the interpretation of the spectra is greatly simplified since the alkali metal atoms are "good" one-electron like systems. Both ionization and harmonic processes are currently under investigation. The results show many similarities with the more extensively studied inert gas atom spectrum but significant differences do exist.

DOI
10.1109/leos.2002.1159540

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In this talk, we will discuss the physics of an alkali metal atom interacting with an intense mid-infrared (3-4 /spl mu/m) laser field. In a Keldysh picture this scaled interaction should show similar ionization dynamics to the more familiar situation of a near visible light interacting with inert gas atoms. However, the interpretation of the spectra is greatly simplified since the alkali metal atoms are "good" one-electron like systems. Both ionization and harmonic processes are currently under investigation. The results show many similarities with the more extensively studied inert gas atom spectrum but significant differences do exist.
We examine strong field atomic physics in a wavelength region (3-4 microns) where very little work has previously been done. The soft photon energy allows the exploration of one-electron atoms with low binding energies (alkali metals). We find that photoionization spectra differ from rare gas studies at shorter wavelengths due to more complex ion core potentials. Harmonic generation is studied, and we find that harmonic bandwidths are consistent with theory and the possibility of compression to pulse widths much shorter than that of the driving pulse. Harmonic yields in the visible and UV are sufficient for a complete study of their amplitude and phase characteristics.
This talk summarizes the results of our microscopic approach to study short-pulse ionization in a many atom system. The interaction of a highly off-resonant light pulse with an atomic gas is modeled fully microscopically. The theory systematically includes the light-atom interaction, as well as the electron-electron and electron-ion interaction effects on the distributions and the optically induced coherent polarization. The resulting equations are solved numerically for an atomic model system excited by a strong light pulse.
Intense laser-matter interactions are at the center of interest in research and technology since the development of high-power lasers.They have been widely used for fundamental studies in atomic, molecular, and optical physics, and they are at the core of attosecond physics and ultrafast optoelectronics.Although the majority of these studies have been successfully described using classical electromagnetic fields, recent investigations based on fully quantized approaches have shown that intense laser-atom interactions can be used for the generation of controllable high-photon-number entangled coherent states and coherent state superpositions.In this tutorial, we provide a comprehensive fully quantized description of intense laseratom interactions.We elaborate on the processes of high-harmonic generation, above-threshold ionization, and we discuss new phenomena that cannot be revealed within the context of semiclassical theories.We provide the description for conditioning the light field on different electronic processes, and their consequences for quantum state engineering of light.Finally, we discuss the extension of the approach to more complex materials, and the impact to quantum technologies for a new photonic platform composed of the symbiosis of attosecond physics and quantum information science.
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.