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Institute of Physics eBooks

Nonlinear light–matter interactions

Thomas Elsaesser, Klaus Reimann, Michael Woerner

Published Sep 1, 2024• 0 citations
Publisher

Abstract

Theoretical concepts and framework for describing nonlinear light-matter interactions are the subject of this chapter. A density matrix approach is introduced for describing the nonlinear optical response of quantum systems to an electromagnetic field. Starting with the full description, different approximations are introduced and their limitations discussed from the viewpoint of physics. Basic concepts such as quantum coherences in multi-level systems, nonlinear currents, and nonperturbative light-matter interactions are explained and illustrated by model calculations.

DOI
10.1088/978-0-7503-6492-8ch3

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Theoretical concepts and framework for describing nonlinear light-matter interactions are the subject of this chapter. A density matrix approach is introduced for describing the nonlinear optical response of quantum systems to an electromagnetic field. Starting with the full description, different approximations are introduced and their limitations discussed from the viewpoint of physics. Basic concepts such as quantum coherences in multi-level systems, nonlinear currents, and nonperturbative light-matter interactions are explained and illustrated by model calculations.
Abstract In this chapter we study with the tools developed in Chapter 3 the basic models that are the foundations of light–matter interaction. We start with Rabi dynamics, then consider the optical Bloch equations that add phenomenologically the lifetime of the populations. As decay and pumping are often important, we cover the Lindblad form, a correct, simple and powerful way to describe various dissipation mechanisms. Then we go to a full quantum picture, quantizing also the optical field. We first investigate the simpler coupling of bosons and then culminate with the Jaynes–Cummings model and its solution to the quantum interaction of a two-level system with a cavity mode. Finally, we investigate a broader family of models where the material excitation operators differ from the ideal limits of a Bose and a Fermi field.
Classical, semi-classical, and quantum-field descriptions for the interaction of light with matter are systematically discussed. Applications of interest include precise determinations of the linear and the non-linear electromagnetic response relevant to resonant pump-probe optical phenomena, such as electromagnetically induced transparency. In the quantum-mechanical description of matter systems, we introduce a general reduced-density-matrix framework. Time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are developed in a unified and self-consistent manner, using a Liouville-space operator representation. A preliminary semi-classical perturbation treatment of the electromagnetic interaction is adopted, in which the electromagnetic field is described as a classical field satisfying the Maxwell equations. Compact Liouville-space operator expressions are derived for the linear and the general (nth order) non-linear electromagnetic-response tensors describing moving many-electron systems. The tetradic matrix elements of the Liouville-space self-energy operators, which are introduced in the time-domain and frequency-domain formulations, are evaluated for environmental collisional and radiative interactions, in order to provide explicit forms for the quantum kinetic equations and the spectral-line shape formulas. It is emphasized that a quantized-field approach is essential for a fully self-consistent quantum-mechanical description of the interacting light-matter system.
Optical generation of high-order harmonics is a prototypical example of nonlinear light–matter interactions in the high-field regime. Quantum optical effects have recently been demonstrated to have a significant influence on this phenomenon. These findings underline the importance of understanding the dynamics of the quantized electromagnetic field during high-order harmonic generation. In the following, we discuss the challenges that are related to the theoretical description of this process and summarize the results that were obtained using the high-field, multimode generalization of well-known quantum optical models that are based on the concept of the two-level atom.
This chapter describes the formation, development, and major subjects of nonlinear optics and photonics. The semiclassical theory treats the light as a classical electromagnetic field governed by Maxwell equations, while the optical medium is a molecular system governed by quantum mechanics; the key parameters for this theory are various-order nonlinear susceptibilities. The quantum theory of radiation treats light as an ensemble of photons and the medium as a molecular system, both of which are described by quantum mechanics, and the key aspect is the concept of the so-called intermediate state represented by a virtual energy state level. The semiclassical theory gives a concise quantitative description of various nonlinear multi-wave mixing effects as well as those nonlinear processes related to the induced refractive-index changes. In contrast, the quantum theory of radiation can provide a conceptual interpretation for almost all known nonlinear optical effects and phenomena.