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Physical Review A

Effect of multiphoton processes on the asymmetric fluorescence spectrum and spectral correlations of a two-level atom driven bichromatically by two strong laser fields

Su-jing Liu, Xu‐xing Geng, Ming Xue, Gao‐xiang Li

Published Oct 6, 2023• 0 citations
Publisher

Abstract

We focus on the influence of multiphoton effect on the fluorescence spectrum and photon statistics of the bichromatically driven two-level atomic system. The influence of the multiphoton effect of the weaker driving field on the system and spontaneous emission are revealed by Schrieffer-Wolff perturbation theory, respectively. The physical origin of the multiphoton process affecting the fluorescence spectral asymmetry characteristics is fully investigated by studying the population distribution and the dressed atomic transition weight. Further, the suppression condition of the central peak of the central band is investigated. The photon statistical properties of the system are revealed by studying the frequency-resolved correlations between different sidepeaks and the central peak and sidepeak, respectively. In particular, the physical picture of the asymmetry of the two-photon correlation signal that is affected by the multiphoton process of the weaker driving field affecting the timing detection is fully revealed by the two methods of correlation moment and conditional quantum state, respectively. These results of ours provide a theoretical approach for studying multiphoton processes in multichromatically driven quantum systems, as well as for developing quantum simulation techniques such as spin locking.

DOI
10.1103/physreva.108.043105

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We focus on the influence of multiphoton effect on the fluorescence spectrum and photon statistics of the bichromatically driven two-level atomic system. The influence of the multiphoton effect of the weaker driving field on the system and spontaneous emission are revealed by Schrieffer-Wolff perturbation theory, respectively. The physical origin of the multiphoton process affecting the fluorescence spectral asymmetry characteristics is fully investigated by studying the population distribution and the dressed atomic transition weight. Further, the suppression condition of the central peak of the central band is investigated. The photon statistical properties of the system are revealed by studying the frequency-resolved correlations between different sidepeaks and the central peak and sidepeak, respectively. In particular, the physical picture of the asymmetry of the two-photon correlation signal that is affected by the multiphoton process of the weaker driving field affecting the timing detection is fully revealed by the two methods of correlation moment and conditional quantum state, respectively. These results of ours provide a theoretical approach for studying multiphoton processes in multichromatically driven quantum systems, as well as for developing quantum simulation techniques such as spin locking.
Abstract Frequency-resolved photon statistics of resonance fluorescence generated from a two-level system driven by a strong laser field and a weak laser field with equal frequencies are studied. The frequency resolution of fluorescent radiation is described by quantum filtering dynamics, which is simulated theoretically by two single-mode quantum optical cavities with tunable frequencies to scan the incident fluorescent radiation. By calculating the two-photon intensity–intensity correlation functions in terms of the cavity modes, we demonstrate that two-color strong correlations of resonance fluorescence can be generated not only between the opposite sidebands, but also between the central band and one of the sidebands: although both sidebands are broadened due to the perturbation of the weak laser field on the strong-field dressed atom. We emphasize that these properties are in contrast to the conventional case of the standard single-atom Mollow triplet. Moreover, if the resonance frequencies of the two filtering cavities are tuned appropriately, broadband two-color strong correlations are predicted, and the physical origin is revealed from the perspective of quantum interference of photon emission dynamics. This can be considered as a feasible scheme for the design of broadband non-classical light sources, and may be beneficial to the quantum precise detection of atomic and molecular dynamics via quantum optical spectroscopy.
We study the fluorescence spectrum of a strongly driven two-level system (TLS) with modulated transition frequency, which is a bichromatically driven TLS and has multiple resonance frequencies. We are aiming to provide a reliable description of the fluorescence in a regime that is difficult to tackle with perturbation theory and the rotating-wave approximation (RWA), and illustrate the spectral features of the fluorescence under off- and multiphoton-resonance conditions. To go beyond the RWA, we use a semianalytical counter-rotating-hybridized rotating-wave method that combines a unitary transformation and Floquet theory to calculate the two-mode Floquet states and quasienergies for the bichromatically driven TLS. We then solve the master equation accounting for the spontaneous decay in the bases of the two-mode Floquet states, and derive a physically transparent fluorescence spectrum. In comparison with the numerically exact spectrum from the generalized Floquet-Liouville approach, the present spectrum is found to be applicable in a wide range of the parameters where the RWA and the secular approximation may break down. We find that the counter-rotating (CR) terms of the transverse field omitted in the RWA have non-negligible contributions to the spectrum under certain conditions. Particularly, at the multiphoton resonance the width of which is comparable with the Bloch-Siegert shift, the RWA and non-RWA spectra markedly differ from each other because of the CR-induced shift. We also analyze the symmetry of the spectrum in terms of the transition matrix elements between the two-mode Floquet states. We show that the strict symmetry of the spectrum cannot be expected without the RWA but the almost symmetric spectrum can be obtained at the single-photon resonance that takes the Bloch-Siegert shift into account if the driving is moderately strong and at the multiphoton resonance with a sufficiently weak transverse field.
Frequency-resolved quantum correlation of resonance fluorescence is investigated in a two-atom radiating system. In this quantum radiating system, only one atom is driven by a laser field, and the spontaneous transition of the undriven atom resonates with one of the Rabi sidebands of the driven atom. A single-mode empty cavity is applied to serve as a Lorentzian filter to output the superbunched fluorescent photon pairs when its frequency is tuned to halfway between the central peak and one of the side peaks. In the case of large filter width, two-photon correlation signal and its physical correspondence can be bridged analytically in our approach. It reveals that this superbunching effect turns out to be the constructive quantum interference between a pair of coupled two-photon cascaded transitions. Ulteriorly, it is the consequence of the modulations of the unfiltered dressed-state transition amplitudes by the filter. Our analytical formalism also shows that, although the dipole-dipole interaction is usually weak, the interatomic coherence caused by this weak perturbation can also play a crucial role in breaking through the superbunching limit obtained from a single two-level atom in the same parameter regime. In addition to being a treasurable quantum pump to probe into the target quantum system, it is also found in our investigation that this superbunched fluorescence can serve as a promising quantum response in detecting this weak perturbation in the interior of the quantum source. A general case is also considered when the two-atom radiating system is monitored by two filter-detector monitoring systems. It is found that this filtered strong quantum correlation can be maintained even though the two photons are spatially separated.
We examine the correlation between photons in the resonance fluorescence of a bichromatically driven four-level atom. The four-level atom consists of two twofold degenerate states and, as a consequence, spontaneous emission events become sensitive to polarization. Depending on the interaction strength with the bichromatic field as well as its polarization direction, nonlinear two-photon emission takes place which, in turn, leads to extremely strong correlations between certain polarized photons. On the other hand, correlations between photons differently polarized from the distinctive ones are suppressed. Thus, the light source establishes a promising candidate for the generation of Bell-type correlated photon pairs. We explain the unusual large correlations with a nonlinear four-photon process which crucially depends on the strength of the driving as well as its polarization.
Frequency-filtered photon correlations have been proven to be extremely useful in grasping how the detection process alters photon statistics. Harnessing the spectral correlations also permits refinement of the emission and unraveling of previously hidden strong correlations in a plethora of quantum-optical systems under continuous-wave excitation. In this work, we investigate such correlations for time-dependent excitation and develop a methodology to compute efficiently time-integrated correlations, which are at the heart of the photon-counting theory, and subsequently apply it to analyze the photon emission of pulsed systems. By combining this formalism with the —which facilitates frequency-resolved correlations—we demonstrate how spectral filtering enhances single-photon purity and suppresses multiphoton noise in time-bin-encoded quantum states. Specifically, filtering the central spectral peak of a dynamically driven two-level system boosts temporal coherence and improves the fidelity of time-bin entanglement preparation, even under conditions favoring multiphoton emission. These results establish spectral filtering as a critical tool for tailoring photon statistics in pulsed quantum light sources.
Abstract This thesis presents an investigation into the quantum characteristics of fluorescence emitted by a two-level atom placed in the electromagnetic vacuum and driven by a classical coherent field. The theoretical analysis employs the Jaynes–Cummings model together with the master-equation formalism commonly used to describe open quantum systems. Within this framework, the work examines key nonclassical fea tures such as photon antibunching, sub-Poissonian statistics, and quantum regression. Particular emphasis is given to resonance fluorescence and the influence of weak and strong driving fields on the coherence properties of the emitted radiation. The master equation is solved in the long-time limit to obtain the evolution of relevant atomic expectation values, which are subsequently used to study population dynamics, mean photon behavior, and spectral features of the fluorescence signal. The study also highlights the role of vacuum fluctuations in spontaneous emission and their impact on the quantum behavior of the atom, ultimately providing insights into the generation of coherent and nonclassical light from driven atomic systems and their relevance to quantum communication and quantum information technologies. Keywords: Fluorescence, Jaynes–Cummings model, Photon statistics, Quantum optics, Two-level atom