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arXiv:2106.02574 · Physical Review Research

Two-photon resonance fluorescence of two interacting nonidentical quantum emitters

Alejandro Vivas-Viaña, Carlos Sánchez Muñoz

Published Aug 10, 2021• 19 citations
arXivHTMLPDF

Abstract

We study a system of two interacting, nonidentical quantum emitters driven by a coherent field. We focus on the particular condition of two-photon resonance and obtain analytical expressions for the stationary density matrix of the system and observables of the fluorescent emission. Importantly, our expressions are valid for the general situation of nonidentical emitters with different transition energies. Our results allow us to determine the regime of parameters in which coherent two-photon excitation, enabled by the coherent coupling between emitters, is dominant over competing, first-order processes. Using the formalism of quantum parameter estimation, we show that the features imprinted by the two-photon dynamics into the spectrum of resonance fluorescence are particularly sensitive to changes in the distance between emitters, making two-photon excitation the optimal driving regime for the estimation of interemitter distance. This can be exploited for applications such as super-resolution imaging of pointlike sources.

DOI
10.1103/physrevresearch.3.033136

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We study a system of two interacting, nonidentical quantum emitters driven by a coherent field. We focus on the particular condition of two-photon resonance and obtain analytical expressions for the stationary density matrix of the system and observables of the fluorescent emission. Importantly, our expressions are valid for the general situation of nonidentical emitters with different transition energies. Our results allow us to determine the regime of parameters in which coherent two-photon excitation, enabled by the coherent coupling between emitters, is dominant over competing, first-order processes. Using the formalism of quantum parameter estimation, we show that the features imprinted by the two-photon dynamics into the spectrum of resonance fluorescence are particularly sensitive to changes in the distance between emitters, making two-photon excitation the optimal driving regime for the estimation of interemitter distance. This can be exploited for applications such as super-resolution imaging of pointlike sources.
Resonance fluorescence of a two-level emitter displays persistently anti-bunching irrespective of the excitation intensity, but inherits the driving laser’s linewidth under weak monochromatic excitation. These properties are commonly explained in terms of two disjoined pictures, i.e., the emitter’s single photon saturation or passively scattering light. Here, we propose a unified model that treats all fluorescence photons as spontaneous emission, one at a time, and can explain simultaneously both the spectral and correlation properties of the emission. We theoretically derive the excitation power dependencies, measurable at the single-photon incidence level, of the first-order coherence of the whole resonance fluorescence and super-bunching of the spectrally filtered, followed by experimental confirmation on a semiconductor quantum dot micro-pillar device. Furthermore, our model explains peculiar coincidence bunching observed in phase-dependent two-photon interference experiments. Our work provides an intuitive understanding of coherent light-matter interaction and may stimulate new applications. Standard descriptions of resonance fluorescence consider either absorption and re-emission in a single-photon picture or passive scattering. This study shows that resonance fluorescence can be described by a pure quantum state of the emitter and photon, revealing a coherent superposition that challenges the conventional view of spontaneous emission as an incoherent process.
Abstract We discuss two-photon correlations from the side peaks that are formed when a two-level system emitter is driven coherently, with a detuning between the driving source and the emitter (quasi-resonance fluorescence). We do so in the context of the theories of frequency-resolved photon correlations and homodyning, showing that their combination leads to a neat picture compatible with perturbative two-photon scattering that was popular in the early days of quantum electrodynamics. This should help to control, enhance and open new regimes of multiphoton emission. We also highlight a way to evidence the quantum coherent nature of the process from photoluminescence only, through the observation of a collapse of the symmetry of the lineshape accompanied by a surge of its intensity of emission. We discuss several of our results in the light of recent experimental works.
Two nonidentical quantum emitters, when placed within a cavity and coherently excited at the two-photon resonance, can reach stationary states of nearly maximal entanglement. In Vivas-Viaña, Martín-Cano, and Sánchez Muñoz [], we introduce a frequency-resolved Purcell effect stabilizing entangled W states among strongly interacting quantum emitters embedded in a cavity. Here we delve deeper into a specific configuration with a particularly rich phenomenology: two interacting quantum emitters under coherent excitation at the two-photon resonance. This scenario yields two resonant cavity frequencies where the combination of two-photon driving and Purcell-enhanced decay stabilizes the system into the subradiant and superradiant states, respectively. By considering the case of nondegenerate emitters and exploring the parameter space of the system, we show that this mechanism is merely one among a complex family of phenomena that can generate both stationary and metastable entanglement when driving the emitters at the two-photon resonance. We provide a global perspective of this landscape of mechanisms and contribute analytical characterizations and insights into these phenomena, establishing connections with previous reports in the literature and discussing how some of these effects can be optically detected. Published by the American Physical Society 2024
Multiphoton emitters are a sought-after resource in quantum photonics. Nonlinear interactions between a multilevel atomic system and a coherent drive can lead to resonant two-photon emission, but harvesting light from this process has remained a challenge due to the small oscillator strengths involved. Here we present a study of two-photon resonance fluorescence at microwave frequencies, using a superconducting, ladder-type artificial atom, a transmon, strongly coupled to a waveguide. We drive the two-photon transition between the ground and second-excited states at increasingly high powers and observe a resonance fluorescence peak whose intensity becomes comparable to single-photon emission until it splits into a Mollow-like triplet. We measure photon correlations of frequency-filtered spectral lines and find that while emission at the fundamental frequency stays antibunched, the resonance fluorescence peak at the two-photon transition is superbunched. Our results provide a route towards the realization of multiphoton sources in the microwave domain.
Numerical simulations of the excitation spectra of resonant fluorescence bound by the dynamic interaction of two different two-level nanoparticles have been performed. We considered the excitation of one of the particles by monochromatic light with a frequency close to the transition frequency of this particle, at an irradiation intensity leading to a small population of its excited state. The formalism for the description of resonance fluorescence by the Heitler--Ma method was applied to a complete compound system of the marked particle pair and quantized emission field. The resulting expressions for the excitation spectrum reflect consideration of the absorption of the fluorescence photon without attributing it to the emission of any one particle. Expressions for the excitation spectra when taking into account such absorption of the fluorescence photon that allows us to attribute it to the radiation of one or another of the particles were obtained by solving a modified system of equations of the Heitler--Ma method, which reflects the addition of non-interfering amplitudes of the emission field states of each particle. It was found that the shape of the excitation spectra of the stationary resonance fluorescence of the particles in question is determined by the shape of the corresponding intensity spectra of the spontaneous fluorescence of these particles. Keywords: mathematical modeling, interacting two-level nanoparticles, resonant fluorescence, excitation spectrum.
In resonance fluorescence excitation experiments, light emitted from solid-state quantum emitters is typically filtered to eliminate the laser photons, ensuring that only red-shifted Stokes photons are detected. However, theoretical analyses of the fluorescence intensity correlation often model emitters as two-level systems, focusing on light emitted exclusively from the purely electronic transition (the zero-phonon line), or they rely on statistical approaches based on conditional probabilities that neglect the quantum coherence between the emitters and the coherence between the electric fields they generate. Here, we propose a model to characterize the correlation of either zero-phonon line photons or Stokes-shifted photons. This model successfully reproduces the experimental correlation of Stokes-shifted photons emitted from two interacting molecules and predicts that this correlation is affected by quantum coherence. Besides, we analyze the role of quantum coherence in the Stokes-shifted emission from two distant emitters, showing a sharp peak at zero time delay due to the Hanbury Brown-Twiss effect.