Abstract Linearity is a fundamental postulate of quantum mechanics which is occasionally the subject of debate. This paper investigates the possibility of checking this assumption by using a laser field. We study the corrections caused by the presence of a small nonlinearity in the Hamiltonian of a quantum system. As a model we use a simplified two-level quantum system whose states are coupled by a small off-diagonal term proportional to the population of the upper level. The nonlinearity causes spontaneous decay of the upper level, shift and broadening of the line and the sensitive dependence of the final state on the initial condition. The presence of a strong laser field, resonant with the atomic transition, enhances the population transfer among the levels and introduces quantitative and qualitative modifications of the spectra of high order harmonic generation (HHG); these are cumulative effects which can be subject to experimental checks. Experiments are needed in order to set an upper limit to the nonlinear term.
Abstract Linearity is a fundamental postulate of quantum mechanics which is occasionally the subject of debate. This paper investigates the possibility of checking this assumption by using a laser field. We study the corrections caused by the presence of a small nonlinearity in the Hamiltonian of a quantum system. As a model we use a simplified two-level quantum system whose states are coupled by a small off-diagonal term proportional to the population of the upper level. The nonlinearity causes spontaneous decay of the upper level, shift and broadening of the line and the sensitive dependence of the final state on the initial condition. The presence of a strong laser field, resonant with the atomic transition, enhances the population transfer among the levels and introduces quantitative and qualitative modifications of the spectra of high order harmonic generation (HHG); these are cumulative effects which can be subject to experimental checks. Experiments are needed in order to set an upper limit to the nonlinear term.
We show that a simple nonperturbative two-level model of an atom driven by a very strong periodic field, results in a rich picture of very high harmonic generation and related phenomena. It reproduces experimentally observed plateau, yields for the first time simple analytic formulas for the plateau cutoff frequency, critical driving intensity, and saturation, and predicts intensity-induced multi-resonances. One of the most fascinating phenomenon discovered recently in nonlinear interaction of light with atoms and ions, is very high-order (up to 135) odd harmonic generation (HHG) by intense (∼ 1013 W/cm2 and higher) optical laser radiation in rare gasses and some ions [1], The spectra of generated harmonics drasticly deviate from the perturbation theory predictions [2], In particular, intensity of harmonics, falling monotonically with their orders only up to a certain point, levels off forming a so-called “plateau", and falls monotonically again beyond it. Generally, harmonte generation depends on phase-matching conditions and nonlinear response of individual atoms. It has recently become clear however [3,4] that the major features of HHG, in particular the plateau, result mainly from general properties of atomic nonlinear response. The most direct and apparently successful way so far to approach the problem theoretically has been numerical simulation of the Schrödinger [2,5-7] (including an empiric rule [6]) for many-electron atoms using Hartry-Slater approximation. This approach requires, however, tremendous amount of calculations and involves many processes, making it difficult to gain simple insights. An interesting simplified model [8] based on 3-D delta-potential with a single (ground) level [9] produces results in integration form. The idea of retaining a single energy scale (ionization energy) brings one close to an even simpler system: a two-level model atom. A two-level model of HHG [10], however, due to various complications introduced into it, failed to generate simple results, whereas an analytic solution [11] holds for a virtually degenerate two-level model only (see below) which is unapplicable to the experimental conditions [1-4,7,9]; besides, no relaxation was considered in [10,11].
Coherent preparation of quantum states of atoms and ions by laser light can lead to electromagnetically induced transparency and related effects. In particular, the standing wave at the adjacent transition induces a new type of nonlinear resonance in the probe-field spectrum of a three-level system. The resonance is due to the effect of high- order harmonics of atomic coherence. However, the resonance is broadened in experiment and the reason of the broadening was unclear. The paper describes how the velocity changing collisions broaden the resonance. The analytic theory taking into account up to 4-th order of the perturbation theory is presented. The numerical solution of density matrix equations is discussed. The analytical formulas are shown to describe the experiment qualitatively while the numerical computation demonstrates quantitative agreement. The Coulomb dephasing is shown to be the physical mechanism of the broadening.
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.
We present a theoretical study of the high-order-harmonic generation (HHG) from coherent superposition states of a three-level system driven by monochromatic cw laser fields. The HHG spectrum can be enhanced by about 105 times via tuning the relative phase between the states which are initially prepared. Even if the ionization effects are taken into account, the enhancement factors are still up to about 102 times. The enhancement is interpreted as the quantum constructive interference of different dipole transitions between quasienergy states. To realize the interference, the intensity of the driving laser field is chosen such that frequencies of the harmonics generated from the different dipole-transition paths, which are dependent on the ac Stark shifted energy separation of quasienergy states, are equal to each other. Moreover, the case studies of HHG spectra from a coherent superposition state of a three-level system show that the enhancement of harmonics is closely related to the harmonic strengths of the dipole transitions, as well as the parity of quasienergy states which are involved in the dipole-transition paths. The reduction of enhancement factors due to ionization effects is also qualitatively analyzed.
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 an analytical framework for the emergence of nonclassical radiation in strongly laser-driven quantum systems, with a focus on high-order harmonic generation (HHG). Starting from a Pauli-Fierz description, we employ a parametric factorization of the coupled light-matter wavefunction that reduces the dynamics to coupled equations for a field-driven electronic state and a quantized light mode. Within this framework, we identify a simple and predictive mechanism for nonclassicality: it originates from the nonlinear dependence of the electronic dipole response on the light-mode coordinate. An approximately constant dipole yields coherent radiation, a linear dependence produces squeezing, and higher-order nonlinearities give rise to Wigner-function negativity. We illustrate this mechanism for atomic and molecular model systems and analyze its scaling in multi-emitter configurations, indicating routes toward high-photon-number nonclassical radiation in HHG. Our results provide a transparent connection between strong-field dynamics and quantum-optical properties of emitted light, offering a basis for engineering nonclassical states in intense laser-matter interactions.