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.
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.
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.
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.
Recent developments on intense laser sources is opening a new field of optical sciences. An intense coherent light beam strongly interacting with the matter causes a coherent motion of a particle, forming a strongly dressed excited particle. A photon emission from this dressed excited particle is a strong nonlinear process causing high-harmonic generation (HHG), where the perturbation analysis is broken down. In this work, we study a coherent photon emission from a strongly dressed excited atom in terms of complex spectral analysis in the extended Floquet-Hilbert-space. We have obtained the eigenstates of the total Hamiltonian with use of Feshbach-Brilloiun-Wigner projection method. In this extended space, the eigenstates of the total Hamiltonian consisting of the radiation field and the atom system have complex eigenvalues whose imaginary part represents the decay rate. Time evolution of the system is represented by the complex eigenvector expansion so that the correlation dynamics between the photon and the atom is fully taken into account. The HHG is interpreted as the irreversible spontaneous photon emission due to the resonance singularity in terms of the multiple Floquet states that are generated by periodic external field. We have found that the interference between the emitted photons over the different Floquet states causes spatial pulse emission correlated with the decay process of the excited atom.
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 nth 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.
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.
High-harmonic generation (HHG) is a prototypical strong-field process in which intense light drives matter to emit radiation at integer multiples of the driving frequency. Extending HHG into the quantum-optical regime offers new opportunities to probe and control strongly nonlinear light-matter interactions using nonclassical states of light. Yet describing this regime requires a fully quantum treatment of the correlated electron-photon dynamics, which becomes computationally challenging for broadband, strongly squeezed fields. Here we solve the quantum-electrodynamical dynamics of a two-level system driven by bright squeezed vacuum in a converged multimode Hilbert space. Both the driving field and emitted harmonics are fully quantized, with the light-matter interaction treated nonperturbatively. This enables direct access to the multimode quantum state and its higher-order correlations beyond semiclassical sampling or perturbative descriptions. We show that squeezed-vacuum driving produces harmonic emission with qualitatively distinct second- and third-order photon correlations compared with coherent excitation. Moreover, back-action from the driven emitter strongly reshapes the incident squeezed field, generating pronounced Wigner-function negativities that evolve on attosecond timescales. Our results establish a fully quantum framework for broadband strong-field dynamics with squeezed light and provide a route to predicting and interpreting quantum-HHG experiments and their extension to more complex emitters.