Due to their conceptual appeal and computational convenience, two‐level systems (TLSs) and generalizations are used to investigate nonlinear behavior in quantum optics and assess the applicability of theoretical methods. Herein, the focus is on second‐harmonic generation (SHG) and, as system of interest, on the Dicke model, which consists of several TLSs inside an optical cavity. The main aspect addressed is the scope of nonequilibrium Green's function (NEGF) to describe the effect of inhomogeneities and electron–electron (e–e) interactions on the SHG signal. For benchmarking purposes, exact diagonalization (ED) results are also presented and discussed. SHG spectra obtained with NEGF and ED are found to be in very good mutual agreement in most situations. Furthermore, inhomogeneity in the TLS and e–e interactions reduce the SHG signal, and the reduction is stronger with inhomogeneity than with interactions. This trend is consistently noted across different (small to large) system sizes. Finally, a modified NEGF approach is proposed to account for cavity leakage, where the quantum photon fields are coupled to a bath of classical oscillators. As expected, within this mixed quantum‐classical scheme, a decrease in the intensity of the fluorescent spectra takes place depending on the entity of leakage.
Due to their conceptual appeal and computational convenience, two‐level systems (TLSs) and generalizations are used to investigate nonlinear behavior in quantum optics and assess the applicability of theoretical methods. Herein, the focus is on second‐harmonic generation (SHG) and, as system of interest, on the Dicke model, which consists of several TLSs inside an optical cavity. The main aspect addressed is the scope of nonequilibrium Green's function (NEGF) to describe the effect of inhomogeneities and electron–electron (e–e) interactions on the SHG signal. For benchmarking purposes, exact diagonalization (ED) results are also presented and discussed. SHG spectra obtained with NEGF and ED are found to be in very good mutual agreement in most situations. Furthermore, inhomogeneity in the TLS and e–e interactions reduce the SHG signal, and the reduction is stronger with inhomogeneity than with interactions. This trend is consistently noted across different (small to large) system sizes. Finally, a modified NEGF approach is proposed to account for cavity leakage, where the quantum photon fields are coupled to a bath of classical oscillators. As expected, within this mixed quantum‐classical scheme, a decrease in the intensity of the fluorescent spectra takes place depending on the entity of leakage.
ABSTRACT Within a cavity quantum electrodynamics framework, we analyse the fluorescent spectrum of ultracold bosons in resonant and second‐harmonic generation (SHG) regimes. Two settings are considered: (i) (few) bosons in an optical lattice and (ii) a trapped two‐component dilute Bose–Einstein condensate (2BEC) within the Bogoliubov scheme. Atom–photon dynamics are treated exactly via time‐dependent configuration interaction, while cavity leakage is modelled via classical oscillator baths. For optical lattices, bosons in short Bose–Hubbard chains with two levels per site show spectral intensity that increases with atom number at weak interactions but decreases and redshifts at strong interactions once atoms outnumber sites. In the 2BEC case, spectra largely scale with particle number when 2BEC–cavity and inter‐particle couplings are rescaled, while strong correlations induce SHG redshifts. These results reveal some generic features of fluorescence in ultracold bosons in optical cavities, and hint at possible experiments and further theoretical developments.
We study the time-resolved fluorescence spectrum in two-level systems interacting with an incident coherent field, both in the weak and intermediate coupling regimes. For a single two-level system in the intermediate-coupling case, as time flows, the spectrum develops distinct features that are not captured by a semiclassical treatment of the incident field. Specifically, for a field on resonance with the atomic transition energy, the usual Mollow spectrum is replaced by a four-peak structure, and for a frequency that is half of the atomic transition energy, the time-dependent spectrum develops a second-harmonic peak with a superimposed Mollow triplet. In the long-time limit, our description recovers results previously found in the literature. After analyzing why a different behavior is observed in the quantum and classical dynamics, the reason for the occurrence of a second-harmonic signal in a two-level system is explained via a symmetry analysis of the total (electron and photon) system and in terms of a three-level system operating in limiting regimes. We find an increased second-harmonic signal in an array of two-level systems, suggesting a superradiance-like enhancement for multiple two-level systems in cavity setups. Finally, initial explorative results are presented for two-level model atoms entering and exiting a cavity, which hint at an interesting interplay between cavity-photon screening and atomic dynamics effects.
Abstract We review one of the most versatile theoretical approaches to the study of time-dependent correlated quantum transport in nano-systems: the non-equilibrium Green’s function (NEGF) formalism. Within this formalism, one can treat, on the same footing, inter-particle interactions, external drives and/or perturbations, and coupling to baths with a (piece-wise) continuum set of degrees of freedom. After a historical overview on the theory of transport in quantum systems, we present a modern introduction of the NEGF approach to quantum transport. We discuss the inclusion of inter-particle interactions using diagrammatic techniques, and the use of the so-called embedding and inbedding techniques which take the bath couplings into account non-perturbatively. In various limits, such as the non-interacting limit and the steady-state limit, we then show how the NEGF formalism elegantly reduces to well-known formulae in quantum transport as special cases. We then discuss non-equilibrium transport in general, for both particle and energy currents. Under the presence of a time-dependent drive—encompassing pump–probe scenarios as well as driven quantum systems—we discuss the transient as well as asymptotic behavior, and also how to use NEGF to infer information on the out-of-equilibrium system. As illustrative examples, we consider model systems general enough to pave the way to realistic systems. These examples encompass one- and two-dimensional electronic systems, systems with electron–phonon couplings, topological superconductors, and optically responsive molecular junctions where electron–photon couplings are relevant.
Long ago, it was predicted that stimulating two-photon processes such as two-photon absorption (TPA) and second harmonic generation (SHG) with entangled photons produced by parametric down-conversion (PDC) could result in higher efficiencies compared to classical illumination [1]. This was experimentally demonstrated for SHG [2] and TPA [3], where, however, the classical comparison was performed by adding losses to the PDC state rather than employing a true classical reference. In addition, these results considered spatially single-mode PDC radiation and were conducted at low photon fluxes, where the PDC modes are, on average, populated by less than one photon. This resulted in an extremely low SHG/TPA signal, considered of limited practical use for metrological applications (such as two-photon fluorescence microscopy or SHG imaging - see, e.g., [4]). A recent theoretical investigation [5] highlighted that a proper analysis of quantum-enhanced two-photon processes requires a fully spatiotemporal model of the nonlinear interactions. It further showed that highly multimode (in space and time) entangled PDC photons can provide a quantum advantage compared to an equivalent classical pulse, even in regimes well beyond the “one-photon-per-mode” limit, considered the boundary of quantum behavior.
We study a generalized Dicke model, as recently realized in an atomic quantum gas experiment, describing the collective interaction of N two-level atoms with a single cavity mode. The model takes account of dissipation of the cavity field, and includes a non-linear atom-photon coupling, not present in the conventional Dicke model. We extend previous theoretical investigations of a semiclassical model by including all quantum effects and considering finite atom number N . Our results show good agreement between quantum expectation values and the semiclassical model as N is increased, but also show exotic behaviour for the corresponding quantum state as the non-linear atom-photon coupling is varied.
We model a collection of N two-level systems (TLSs) coupled to a multimode cavity via Meyer-Miller-Stock-Thoss (MMST) dynamics, sampling both electronic and photonic zero-point energies (ZPEs) and propagating independent trajectories in Wigner phase space. By investigating the ground-state stability of a single TLS, we use MMST dynamics to separately study both electronic ZPE effects (which would naively lead to the breakdown of the electronic ground state) and photonic ZPE effects (which would naively lead to spontaneous absorption). By contrast, including both effects, i.e., sampling both electronic and photonic ZPEs, leads to the dynamical stability of the electronic ground state. Therefore, MMST dynamics provides a practical way to identify the contributions of self-interaction and vacuum fluctuations. More importantly, we find that MMST dynamics can predict accurate quantum dynamics for both electronic populations and electromagnetic field intensity in the high saturation limit. For a single TLS in a cavity, MMST dynamics correctly predicts the initial exponential decay of spontaneous emission, Poincar\'e recurrences, and the positional dependence of a spontaneous emission rate. For an array of N equally spaced TLSs with only one TLS excited initially, MMST dynamics correctly predicts the modification of spontaneous emission rate as a function of the spacing between TLSs. Finally, MMST dynamics also correctly models Dicke's superradiance and subradiance, i.e., the dynamics when all TLSs are excited initially, including the correct quantum statistics for the delay time (as found by counting trajectories, for which a full quantum simulation is hard to achieve). Therefore, this work raises the possibility of simulating large-scale collective light-matter interactions with methods beyond mean-field theory.