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arXiv:2311.01726 · Physical Review A

Parametric model for high-order harmonic generation with quantized fields

Ákos Gombkötő, Sándor Varró, B.G. Pusztai, István Magashegyi, Attila Czirják, Szabolcs Hack, Péter Földi

Published May 20, 2024• 4 citations
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Abstract

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 $n\mathrm{th}$ harmonic mode are created during the annihilation of $n$ 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.

DOI
10.1103/physreva.109.053717

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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.
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.
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.
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.
We present a study of photon statistics associated with high-order harmonic generation (HHG) involving one-mode and intermodal correlations of the high harmonic photons. The aim of the paper is to give insight into the nonclassical properties of high-order harmonic modes. To this end, we use a simplified model describing an elementary quantum emitter: the model of a two-level atom. While the material system is extremely simplified in this description, the conclusions and the methods may be generalized for more complex cases. Our primary interest is an effective model of HHG in which the exciting pulse is classical and the harmonics are quantized, although we touch upon the more generalized, fully quantized model as well. Evolution of the Mandel parameter, photon antibunching, squeezing, and cross correlations are calculated. Results imply that with respect to a single quantized emitter, nonclassicality of the harmonics is present: sub-Poissonian photon statistic and squeezing can characterize certain optical modes, while strong anticorrelation can also be present.
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.
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.