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Two-photon spectra of quantum emitters

Alejandro González-Tudela, Materia Condensada, Fabrice P. Laussy, C. Tejedor, Michael J. Hartmann, Elena del Valle

Published Jan 1, 2013• 96 citations
OpenAlex

Abstract

Abstract. We apply our recently developed theory of frequency-filtered and time-resolved N-photon correlations [1] to study the two-photon spectra of a variety of systems of increasing complexity: single mode emitters with two limiting statistics (one harmonic oscillator or a two-level system) and the various combinations that arise from their coupling. We consider both the linear and nonlinear regimes under incoherent excitation. We find that even the simplest systems display a rich dynamics of emission, not accessible by simple single photon spectroscopy. In the strong coupling regime, novel two-photon emission processes involving virtual states are revealed. Furthermore, two general results are unraveled by two-photon correlations with narrow linewidth detectors: i) filtering induced bunching and ii) breakdown of the semi-classical theory. We show how to overcome this shortcoming in a fully-quantized picture. PACS numbers: 42.50.Ar,42.50.Lc,05.10.Gg,42.25.Kb,42.79.Pw ar X iv

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Abstract. We apply our recently developed theory of frequency-filtered and time-resolved N-photon correlations [1] to study the two-photon spectra of a variety of systems of increasing complexity: single mode emitters with two limiting statistics (one harmonic oscillator or a two-level system) and the various combinations that arise from their coupling. We consider both the linear and nonlinear regimes under incoherent excitation. We find that even the simplest systems display a rich dynamics of emission, not accessible by simple single photon spectroscopy. In the strong coupling regime, novel two-photon emission processes involving virtual states are revealed. Furthermore, two general results are unraveled by two-photon correlations with narrow linewidth detectors: i) filtering induced bunching and ii) breakdown of the semi-classical theory. We show how to overcome this shortcoming in a fully-quantized picture. PACS numbers: 42.50.Ar,42.50.Lc,05.10.Gg,42.25.Kb,42.79.Pw ar X iv
We apply our recently developed theory of frequency-filtered and time-resolved N -photon correlations (del Valle et al 2012 Phys. Rev. Lett. 109 183601) to study the two-photon spectra of a variety of systems of increasing complexity: single-mode emitters with two limiting statistics (one harmonic oscillator or a two-level system) and the various combinations that arise from their coupling. We consider both the linear and nonlinear regimes under incoherent excitation. We find that even the simplest systems display a rich dynamics of emission, not accessible by simple single-photon spectroscopy. In the strong coupling regime, two-photon emission processes involving virtual states are revealed. Furthermore, two general results are unravelled by two-photon correlations with narrow linewidth detectors: (i) filtering-induced bunching and (ii) breakdown of the semi-classical theory. We show how to overcome the latter in a fully quantized picture.
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.
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.
Accessing complete information about the emission from any quantum-optical systems requires tools capable of a frequency-resolved characterization of multi-photon transitions that would go beyond the standard g(2) correlation measurements. This is particularly important when analyzing systems which exhibit strong nonlinear response with multiple emission pathways. In this work, we calculate and analyze in details correlations of light emitted from two such canonical nonlinear optical systems, one incorporating Kerr nonlinear medium, and another exhibiting optomechanical coupling between light and quantized motion of a generic mechanical oscillator. We compare their single- and two-photon emission characteristics by employing a recently developed framework that allows us to calculate the frequency-resolved g(2) correlations between emitted photons with two arbitrary frequencies. Our analysis shows a rich landscape of bunching and antibunching associated with multi-photon emission events, and reveals the distinctive temporal characteristics of such processes. This new understanding provides a new asset to characterize and exploit nonlinear phenomena in Kerr and optomechanical systems in future experiments.
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.
Frequency-resolved photon emission is central to applications from quantum information encoding to high-resolution spectroscopy, and then studying their correlations is therefore essential for revealing the underlying emission pathways and multiphoton statistics. Here, we investigate frequency-resolved N-photon correlations in an ultrastrongly coupled cavity QED system where a qubit interacts with a single-mode cavity. Owing to counter-rotating interactions, the eigenstates and energy spectrum are strongly modified, giving rise to rich spectral and statistical properties in the emitted frequency-resolved photons. Through frequency-selective detection, we reveal pronounced multiphoton antibunching, as well as multiphoton bunching originating from cascade transitions among dressed eigenstates. In particular, we show that parity symmetry plays a decisive role in shaping these correlations. The symmetry-breaking opens additional transition channels and dramatically enhances the generation of correlated photon pairs and even photon triplets of different frequencies. Our work extends frequency-resolved correlations to the ultra-strong coupling regime and demonstrates their potential as a sensitive probe of symmetry in light-matter interaction systems.