The quantum optical description of high-order harmonic generation where both the electrons of the generating medium and the driving and generated light fields are described quantum mechanically has been of significant interest in the past years. The quantum optical formulation leads to equations of motion for the generated light field in which the quantum optical field couples to the time-dependent current of the electronic medium irrespectively of the specifics of the electronic system being an atom, molecule, or solid. These equations of motion are not solvable for any realistic system and accurate and verified approximations are hence needed. In this paper, we present a hierarchy of approximations for the equations of motion for the photonic state. At each level in this hierarchy, we compare it to the previous level justifying the validity using the Fermi-Hubbard model as an example of an electronic system with correlations. This model allows us to perform an accurate simulation of the electron motion of all the required states. We find that for the typical experimental situation of weak quantized-light-matter-coupling constant and at intensities well below the damage threshold, an explicit expression for the generated quantum light, referred to as the Markov-state approximation, captures the high-harmonic spectrum quantitatively and describes the single-mode quantum properties of the generated light as characterized by the Mandel-$Q$ parameter and the degree of squeezing qualitatively.
The quantum optical description of high-order harmonic generation where both the electrons of the generating medium and the driving and generated light fields are described quantum mechanically has been of significant interest in the past years. The quantum optical formulation leads to equations of motion for the generated light field in which the quantum optical field couples to the time-dependent current of the electronic medium irrespectively of the specifics of the electronic system being an atom, molecule, or solid. These equations of motion are not solvable for any realistic system and accurate and verified approximations are hence needed. In this paper, we present a hierarchy of approximations for the equations of motion for the photonic state. At each level in this hierarchy, we compare it to the previous level justifying the validity using the Fermi-Hubbard model as an example of an electronic system with correlations. This model allows us to perform an accurate simulation of the electron motion of all the required states. We find that for the typical experimental situation of weak quantized-light-matter-coupling constant and at intensities well below the damage threshold, an explicit expression for the generated quantum light, referred to as the Markov-state approximation, captures the high-harmonic spectrum quantitatively and describes the single-mode quantum properties of the generated light as characterized by the Mandel-Q parameter and the degree of squeezing qualitatively.
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.
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.
In recent years, strong-field processes such as high-order harmonic generation (HHG) and above-threshold ionization driven by nonclassical states of light have become an increasingly popular field of study. The theoretical modeling of these processes often applies an approximate phase-space expansion of the nonclassical driving field in terms of coherent states, which has been shown to accurately predict the harmonic spectrum. However, its accuracy for the computation of quantum optical observables like the degree of squeezing and photon statistics has not been thoroughly considered. In this work, we introduce this approximative phase-space description and discuss its accuracy, and we find that it mischaracterizes the quantum optical properties of the driving laser by making it an incoherent mixture of classical states. We further show that this error in the driving field description maps onto the light emitted from HHG, as neither sub-Poissonian photon statistics nor quadrature squeezing below vacuum fluctuations can be captured by the approximative phase-space description. Lastly, to benchmark the approximative phase-space description, we consider the quantum HHG from a one-band model, which yields an exact analytical solution. Using the approximative phase-space representation with this specific model, we find a small quantitative error in the quadrature variance of the emitted field that scales with pulse duration and emitter density. Our results show that using this approximative phase-space description can mischaracterize quantum optical observables. Attributing physical meaning to such results should therefore be accompanied by a quantitative analysis of the error.
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.
We study the effect of electron-electron correlations on the quantum state of the light emitted from high-harmonic generation (HHG). The quantum state of the emitted light is obtained by using a fully quantum mechanical description of both the optical modes as well as the electronic system. This is different from the usual semiclassical description of HHG, which only treats the electronic target system quantum mechanically. Using the generic Fermi-Hubbard model, the strength of the electron-electron correlation can be treated as a parameter enabling us to investigate the two limiting cases of a completely uncorrelated phase and a correlated Mott-insulating phase. In the completely uncorrelated phase, the model reduces to a single-band tight-binding model in which only intraband currents contribute to the spectrum. In this limit, we analytically find that the emitted light is in a classical coherent state. In the Mott-insulating phase, a consideration of the photon statistics and squeezing of the emitted photonic state shows that the inter-Hubbard-subband current generates nonclassical light. In this sense, we show that electron-electron correlation can induce the generation of nonclassical states of light.
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.