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arXiv:1910.09894 · Physical Review A

High-order harmonic generation as induced by a quantized field: Phase-space picture

Ákos Gombkötő, Sándor Varró, Péter Mati, Péter Földi

Published Jan 13, 2020• 36 citations
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Abstract

The interaction of matter with a quantized electromagnetic mode is considered. Representing a strong exciting field, the mode is assumed to contain a large number of photons. As a result, the material response is highly nonlinear: the completely quantized description results in generation of high harmonics. In order to understand the essence of the physical processes that are involved, we consider a finite dimensional model for the material system. Using an appropriate description in phase space, this approach leads to a transparent picture showing that the interaction splits the initial, exciting coherent state into parts, and the rapid change of the populations of these parts (that are coherent states themselves) results in the generation of high-order harmonics as secondary radiation. The method we use is an application of the discrete lattice of coherent states that was introduced by von Neumann.

DOI
10.1103/physreva.101.013418

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The interaction of matter with a quantized electromagnetic mode is considered. Representing a strong exciting field, the mode is assumed to contain a large number of photons. As a result, the material response is highly nonlinear: the completely quantized description results in generation of high harmonics. In order to understand the essence of the physical processes that are involved, we consider a finite dimensional model for the material system. Using an appropriate description in phase space, this approach leads to a transparent picture showing that the interaction splits the initial, exciting coherent state into parts, and the rapid change of the populations of these parts (that are coherent states themselves) results in the generation of high-order harmonics as secondary radiation. The method we use is an application of the discrete lattice of coherent states that was introduced by von Neumann.
Abstract Traditionally, the theoretical description of the optical generation of high-order harmonics relies on the semiclassical approximation, i.e., on the assumption that the exciting radiation (driving) can be treated as a classical, time-dependent field. Recent results, however, show that the quantized nature of the electromagnetic radiation (”photon picture”) plays a significant, experimentally observable role in the process. Along this line, in this work we describe a general model, in which both the exciting field and the high harmonic modes are quantized, while the target material appears via parameters only. The time evolution of the quantized field modes clearly shows gradually increasing population of the harmonics at the expense of decreasing photon numbers in the excitation. The process is visualized in the phase-space, using Wigner functions.
A quantum optical model for high-order harmonic generation is presented in which both the exciting field and the high-order harmonic modes are quantized, while the target material appears only via parameters. As a consequence, the model is independent of the excited material system to a large extent and allows us to focus on the properties of the electromagnetic fields. Technically, the Hamiltonian known for parametric down-conversion is adopted, where photons in the nthn\mathrm{th}nth harmonic mode are created during the annihilation of nnn photons from the fundamental mode. In our treatment, initially, the fundamental mode is in a coherent state corresponding to large photon numbers, while the high-order harmonic modes are in vacuum state. Due to the interaction, the latter modes get populated while the fundamental one loses photons. Analytical approximations are presented for the time evolution that are verified by numerically exact calculations. For multimode, finite-bandwidth excitation, the time dependence of the high-order harmonic radiation is also given.
Studies of high harmonic generation (HHG) have entered a new stage by using the quantum light instead of the classical field. Recent theoretical progress has demonstrated promising features, such as the significantly higher maximum harmonic photon energy in a squeezed or thermal light field, which is not observed under classical field conditions with the same number of fundamental mode photons. However, there are many approximations in the theoretical treatments. More accurate methods are required to check the appealing results. By employing the generalized von Neumann lattice basis, here we develop a general and precise method to describe the HHG process, taking into account the coherent superposition of the diagonal part components and the nondiagonal part components from the overlap of the coherent states. It can be extended to calculate the multimode quantum light, such as two-mode squeezed vacuum. Our study provides a powerful tool for investigating the full properties of quantum light in HHG.
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.
Quantum-optical descriptions of strong-field processes have attracted significant attention in recent years. Typically, the theoretical modeling has been conducted in the Schrödinger picture, where results are only obtainable under certain approximations, while, in contrast, the Heisenberg picture has remained relatively unexplored. In this work, we develop an accurately controlled perturbative expansion of the time-evolution operator in the Heisenberg picture and derive beyond-semiclassical corrections to the emitter dynamics due to the coupling to the quantized electromagnetic field, capturing effects of the quantum fluctuations present in the latter. We focus on high-order harmonic generation (HHG), where the approach is accurate in parameter regimes of current interest and it gives closed-form expressions for key observables. This formulation not only simplifies numerical calculations compared to the Schrödinger-picture approach but also provides a clear correspondence between nonclassical features of the emitted light and the underlying induced dynamics of the generating medium including quantum fluctuations. Moreover, the Heisenberg framework naturally yields scaling relations with the number of independent emitters, enabling us to assess whether nonclassical behavior should persist under typical experimental conditions involving large emitter ensembles. Interestingly, we find that the degree of squeezing increases with the number of emitters, whereas the photon statistics approaches a classical Poissonian distribution in the many-emitter limit. We also find that the beyond-semiclassical emitter dynamics significantly enhances the degree of squeezing of the emitted light. Our work advances the theoretical understanding of quantum-optical HHG and introduces an accessible and well-controlled framework to describe realistic experiments.
We investigate a two-level atom in the field of a strong laser pulse. The resulting time-dependent polarization is the source of a radiation the frequency components of which are essentially harmonics of the driving field's carrier frequency. The time evolution of this secondary radiation is analyzed in terms of the expectation values of the photon-number operators for a large number of electromagnetic modes that are initially in the vacuum state. Our method is based on a multimode version of the Jaynes-Cummings-Paul model and can be generalized to different radiating systems as well. We show that, after the exciting pulse, the final distribution of the photon numbers is close to the conventional (Fourier-transform-based) power spectrum of the secondary radiation. The details of the high-order-harmonic spectra (HHG spectra) are also analyzed; for many-cycle excitations a clear physical interpretation is given in terms of the Floquet quasienergies. A first step towards the determination of the photon statistics of the high-order-harmonic modes reveals states with slightly super-Poissonian distribution.