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arXiv:2302.09020 · Physical Review A

Resonance fluorescence of two asymmetrically pumped and coupled two-level systems

Charles Andrew Downing, Elena del Valle, Antonio I. Fernández‐Domínguez

Published Feb 17, 2023• 7 citations
arXivHTMLPDF

Abstract

We study a driven-dissipative duo of two-level systems in an open quantum systems approach, modeling a pair of atoms or (more generally) meta-atoms. Allowing for complex-valued couplings in the setup, which are of both a coherent and incoherent character, gives rise to a diverse coupling landscape. We consider several points on this landscape, for example where the coupling between the two coupled two-level systems is dominated by coherent, incoherent, unsymmetrical, and even unidirectional interactions. Traversing the coupling terrain leads to remarkable features in the populations of the pair, correlations, and optical spectra. Most notably, the famous Mollow triplet spectrum for a single atom may be superseded for a pair by a Mollow quintuplet (or even by a spectral singlet) and the setup allows for population trapping to arise, all depending upon the precise nature of the coupling between the two-level systems.

DOI
10.1103/physreva.107.023717

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We study a driven-dissipative duo of two-level systems in an open quantum systems approach, modeling a pair of atoms or (more generally) meta-atoms. Allowing for complex-valued couplings in the setup, which are of both a coherent and incoherent character, gives rise to a diverse coupling landscape. We consider several points on this landscape, for example where the coupling between the two coupled two-level systems is dominated by coherent, incoherent, unsymmetrical, and even unidirectional interactions. Traversing the coupling terrain leads to remarkable features in the populations of the pair, correlations, and optical spectra. Most notably, the famous Mollow triplet spectrum for a single atom may be superseded for a pair by a Mollow quintuplet (or even by a spectral singlet) and the setup allows for population trapping to arise, all depending upon the precise nature of the coupling between the two-level systems.
We study a prototypical model of two coupled two-level systems, where the competition between coherent and dissipative coupling gives rise to a rich phenomenology. In particular, we analyze the case of asymmetric coupling, as well as the limiting case of chiral (or one-way) coupling. We investigate various quantum optical properties of the system, including its steady-state populations, power spectrum, and second-order correlation functions, and outline the characteristic features which emerge in each quantity as one sweeps through the nontrivial landscape of effective complex couplings. Most importantly, we reveal instances of population trapping, unexpected spectral features, and strong emission correlations.
We present an open-system master equation study of the coherent and incoherent resonance fluorescence spectrum from a two-level quantum system under coherent pulsed excitation. Several pronounced features that differ from the fluorescence under a constant drive are highlighted, including a multi-peak structure and a pronounced off-resonant spectral asymmetry, in stark contrast to the conventional symmetrical Mollow triplet. We also study semiconductor quantum dot systems using a polaron master equation and show how the key features of dynamic resonance fluorescence change with electron-acoustic-phonon coupling.
A cavity-modified master equation is derived for a coherently driven two-level atom coupled to a single-mode cavity in the bad cavity limit, in which the cavity frequency is tuned to either the center or one of the sidebands of the Mollow triplet. The atomic populations in both the bare- and dressed-state representations are analyzed in terms of the cavity-modified transition rates. In the bare-state basis, the role of the cavity may be interpreted as enhancing the stimulated absorption of the atom while suppressing the stimulated emission. The bare-state population may thus be inverted under appropriate conditions. The dressed-state inversion, however, originates from the enhancement of the atom-cavity interaction when the cavity is resonant with the atomic dressed-state transition. We show that two-phase quadratures of the atomic polarization decay at different rates. The decay of the in-phase (or out-of-phase) quadrature may be greatly inhibited as the driving intensity increases, depending on the cavity resonant frequency. The spectrum of the atomic fluorescence emitted out the side of the cavity is also studied. The spectral profiles are sensitive to the cavity frequency. When the cavity frequency is tuned to the center of the Mollow resonances, the fluorescence spectrum is symmetrical with three peaks whose linewidths and heights are intensity dependent. When the cavity frequency is tuned to one of the Mollow sidebands, however, it is asymmetric, and the central peak and the sideband on resonance with the cavity can be significantly suppressed for strong driving fields. All three spectral lines can be narrowed by increasing the Rabi frequency. The physics of these striking spectral features is explored in the dressed-state basis. We also investigate the probe absorption spectrum. When the cavity frequency is tuned to the center of the Mollow fluorescence triplet, the central component exhibits a Lorentzian line shape, while the side bands show the Rayleigh-wing line shape. Probe gain may occur at line center due to cavity-induced, bare-state population inversion. When the cavity is tuned to resonance with one sideband, only two sidebands, with Lorentzian profiles, dominate. Gain can occur at the sideband far off resonant with the cavity. The sideband gain is a consequence of an unbalanced dressed-state population distribution.
We calculate the steady-state spectrum of resonance fluorescence from a two-level atom coupled to a single cavity mode and driven by a strong, in general off-resonance, external field. In the strong-coupling limit, each Mollow triplet component is split into a multiplet, whose detailed structure depends on the atom–cavity coupling, the cavity and spontaneous emission decay constants, and the photon-number distribution of the cavity mode. The dressed states for this system are identified, and the spectral features are interpreted in terms of transitions among these dressed states. In particular, we find that the central component of the central multiplet can have a strongly subnatural linewidth.
The coherent interaction between a two-level system and electromagnetic fields serves as a foundation for fundamental quantum physics and modern photonic quantum technology. A profound example is resonance fluorescence, where the non-classical photon emission appears in the form of a Mollow-triplet when a two-level system is continuously driven by a resonant laser. Pushing resonance fluorescence from a static to dynamic regime by using short optical pulses generates on-demand emissions of highly coherent single photons. Further increasing the driving strength in the dynamical regime enables the pursuit of exotic non-classical light emission in photon number superposition, photon number entanglement, and photon bundle states. However, the long-sought-after spectrum beyond the Mollow-triplet, a characteristic of dynamic resonance fluorescence under strong driving strength, has not been observed yet. Here we report the direct observation and systematic investigations of dynamic resonance fluorescence spectra beyond the Mollow-triplet in a solid-state cavity quantum electrodynamic system. The dynamic resonance fluorescence spectra with up to five pairs of side peaks, excitation detuning induced spectral asymmetry, and cavity filtering effect are observed and quantitatively modeled by a full quantum model with phonon scattering included. Time-resolved measurements further reveal that the multiple side peaks originate from interference of the emission associated with different temporal positions of the excitation pulses. Our work facilitates the generation of a variety of exotic quantum states of light with dynamic driving of two-level systems.
We investigate cooperative fluorescence in a dilute cloud of strongly driven two-level emitters. Starting from the Heisenberg equations of motion, we compute the first-order scattering corrections to the saturation of the excited-state population and to the resonance-fluorescence spectrum, which both require going beyond the state-of-the-art linear-optics approach to describe collective phenomena. A dipole blockade is observed due to long-range dipole-dipole coupling that vanishes at stronger driving fields. Furthermore, we compute the inelastic component of the light scattered by a cloud of many atoms and find that the Mollow triplet is affected by cooperativity. In a lobe around the forward direction, the inelastic Mollow triplet develops a spectral asymmetry, observable under experimental conditions.