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arXiv:2504.11294

On the Relationship Between Antibunching and Entanglement in Resonance Fluorescence

Xinxin Hu, Gabriele Maron, Luke Masters, Arno Rauschenbeutel, Jürgen Volz

Published Apr 15, 2025• 0 citations
arXivHTMLPDF

Abstract

Photon antibunching in resonance fluorescence - the emission from a single, resonantly driven two-level quantum emitter - is a paradigmatic signature of nonclassical light. Photon entanglement, by contrast, manifests as correlations that can defy any classical description and is typically regarded as a distinct quantum effect. Here, we experimentally extract pairs of narrowband, time-bin-entangled photons from the antibunched resonance fluorescence of a single trapped atom. We verify entanglement via violation of the CHSH Bell inequality and by reconstructing the two-photon density matrix. The observed correlations vanish when the coincidence time window exceeds the antibunching timescale, revealing underlying multimode entanglement in the emitted field. Our results establish a direct link between photon antibunching and photon-photon entanglement, unifying two canonical signatures of nonclassical light.

DOI
10.48550/arxiv.2504.11294

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Photon antibunching in resonance fluorescence - the emission from a single, resonantly driven two-level quantum emitter - is a paradigmatic signature of nonclassical light. Photon entanglement, by contrast, manifests as correlations that can defy any classical description and is typically regarded as a distinct quantum effect. Here, we experimentally extract pairs of narrowband, time-bin-entangled photons from the antibunched resonance fluorescence of a single trapped atom. We verify entanglement via violation of the CHSH Bell inequality and by reconstructing the two-photon density matrix. The observed correlations vanish when the coincidence time window exceeds the antibunching timescale, revealing underlying multimode entanglement in the emitted field. Our results establish a direct link between photon antibunching and photon-photon entanglement, unifying two canonical signatures of nonclassical light.
Resonance fluorescence, the process in which a single two-level quantum emitter interacts with a near-resonant coherent light, is a cornerstone of quantum optics as a paradigmatic light-matter interaction. Quantum phenomena in resonance fluorescence have been accounted for in terms of one- and two-photon processes; however, the physical processes arising from the interaction of a single two-level atom with higher photon numbers remain unexplored experimentally. Here we experimentally reveal the multiphoton scattering nature of resonance fluorescence, which intrinsically gives rise to multiphoton entanglement. By accessing quantum fluctuations in the field emitted from a cavity-quantum electrodynamics system, we resolve third- and fourth-order photon scattering events from a single two-level atom. In the three-photon component, the scattered photons are shown to be genuinely energy-time entangled, as verified by a violation of Svetlichny's inequality. As a demonstration of an application, a quantum secret sharing protocol (QSS) is implemented using this entangled photon source. Our study refines the descriptive framework of resonance fluorescence and broadens the scope of its investigation. It also establishes a fundamentally simple route for generating multiphoton entangled states for quantum information processing and quantum metrology.
Resonance fluorescence from a coherently driven two-level emitter is a minimal quantum optical field that combines phase coherence with single-photon-level nonlinearity. Here we show that it can be engineered, using only passive linear interferometry, into energy-time entanglement. By injecting resonance fluorescence from a single quantum dot into an asymmetric Mach--Zehnder interferometer operated near destructive interference of the single-photon component, we generate an output field whose coincidence statistics are dominated by the simultaneous two-photon contribution |2> and the temporally separated photon-pair contribution |11>. In a Franson geometry, these two sectors are resolved on the coincidence-delay axis, and both exhibit high-visibility nonlocal interference fringes and violate the Clauser--Horne--Shimony--Holt Bell inequality. Our results reveal a general route for engineering entanglement from resonance fluorescence using passive optics.
Resonance fluorescence has played a major role in quantum optics with predictions and later experimental confirmation of nonclassical features of its emitted light such as antibunching or squeezing. In the Rayleigh regime where most of the light originates from the scattering of photons with subnatural linewidth, antibunching would appear to coexist with sharp spectral lines. Here, we demonstrate that this simultaneous observation of subnatural linewidth and antibunching is not possible with simple resonant excitation. Using an epitaxial quantum dot for the two-level system, we independently confirm the single-photon character and subnatural linewidth by demonstrating antibunching in a Hanbury Brown and Twiss type setup and using high-resolution spectroscopy, respectively. However, when filtering the coherently scattered photons with filter bandwidths on the order of the homogeneous linewidth of the excited state of the two-level system, the antibunching dip vanishes in the correlation measurement. Our observation is explained by antibunching originating from photon-interferences between the coherent scattering and a weak incoherent signal in a skewed squeezed state. This prefigures schemes to achieve simultaneous subnatural linewidth and antibunched emission.
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.
We investigate two-color photon correlations in the light emitted by two strongly driven, strongly interacting two-level emitters. The correlations are interpreted introducing the collective dressed states picture, which allows us to describe both bunching and antibunching based on the allowed and prohibited transitions. At odds from weakly interacting emitters, the strong interaction lifts the degeneracy of the energy differences between the different states, leading to a temporal breaking of symmetry for the correlations: photons of different frequencies may not be emitted in any order. Finally, we show that most of the virtual processes, which involve pairs of photons, yield nonclassical correlations when the sum of their energies fits any of the interaction-induced sidebands in the emitted spectrum. In particular, depending on the frequency of the emitted photons, correlations strong enough to violate Bell inequalities can appear.
Abstract Resonance fluorescence—the light emitted when exciting resonantly a two-level system—is a popular quantum source as it seems to inherit its spectral properties from the driving laser and its statistical properties from the two-level system, thus providing a subnatural-linewidth single-photon source (SPS). However, these two qualities do not actually coexist in resonance fluorescence, since an optical target detecting these antibunched photons will either be spectrally broad itself and not benefit from the spectrally narrow source, or match spectrally with the source but in this case the antibunching will be spoiled. We first explain this failure through a decomposition of the field-emission and how this gets affected by frequency resolution. We then show how to restore the sought joint subnatural linewidth and antibunched properties, by interfering the resonance fluorescence output with a coherent beam. We finally discuss how the signal that is eventually generated in this way features a new type of quantum correlations, with a plateau of antibunching which suppresses much more strongly close photon pairs. This introduces a new concept of perfect SPS.