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Nature Photonics

On the simultaneous scattering of two photons by a single two-level atom

Luke Masters, Xinxin Hu, Martin Cordier, Gabriele Maron, Lucas Pache, Arno Rauschenbeutel, Max Schemmer, Jürgen Volz

Published Jul 27, 2023• 32 citations
Publisher

Abstract

Abstract The interaction of light with a single two-level emitter is the most fundamental process in quantum optics, and is key to many quantum applications. As a distinctive feature, two photons are never detected simultaneously in the light scattered by the emitter. This is commonly interpreted by saying that a single two-level quantum emitter can only absorb and emit single photons. However, it has been theoretically proposed that the photon anticorrelations can be thought of as arising from quantum interference between two possible two-photon scattering amplitudes, which one refers to as coherent and incoherent. This picture is in stark contrast to the aforementioned one, in that it assumes that the atom has two different mechanisms at its disposal to scatter two photons at the same time. Here we experimentally validate the interference picture by showing that, when spectrally rejecting only the coherent component of the fluorescence light of a single two-level atom, the remaining light consists of photon pairs that have been simultaneously scattered by the atom. Our results offer fundamental insights into the quantum-mechanical interaction between light and matter and open up novel approaches for the generation of highly non-classical light fields enabling, for example, Fourier-limited photon-pair sources that approach the theoretical limit in brightness.

DOI
10.1038/s41566-023-01260-7

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Abstract The interaction of light with a single two-level emitter is the most fundamental process in quantum optics, and is key to many quantum applications. As a distinctive feature, two photons are never detected simultaneously in the light scattered by the emitter. This is commonly interpreted by saying that a single two-level quantum emitter can only absorb and emit single photons. However, it has been theoretically proposed that the photon anticorrelations can be thought of as arising from quantum interference between two possible two-photon scattering amplitudes, which one refers to as coherent and incoherent. This picture is in stark contrast to the aforementioned one, in that it assumes that the atom has two different mechanisms at its disposal to scatter two photons at the same time. Here we experimentally validate the interference picture by showing that, when spectrally rejecting only the coherent component of the fluorescence light of a single two-level atom, the remaining light consists of photon pairs that have been simultaneously scattered by the atom. Our results offer fundamental insights into the quantum-mechanical interaction between light and matter and open up novel approaches for the generation of highly non-classical light fields enabling, for example, Fourier-limited photon-pair sources that approach the theoretical limit in brightness.
The interaction of light with a two-level emitter is the most fundamental process in quantum optics and key to many applications in quantum science and technology. One peculiarity is that two photons are never simultaneously detected in the light scattered by a single quantum emitter. This is commonly interpreted to mean that a single two-level quantum emitter can only absorb and emit single photons. Here we show by spectrally filtering the fluorescence of such an emitter, that the remaining light consists of a stream of photon pairs that have been simultaneously scattered by the two-level emitter [1].
Resonance fluorescence from a two-level emitter is a standard route to single-photon generation, where the emitter produces only one photon at a time, and multiphoton emission or scattering is inherently suppressed. In this study, we challenge this paradigm in the weak-excitation limit, where coherent scattering dominates. Using a single quantum dot in a microcavity, we show that the incoherent component exhibits pronounced superbunching, revealing simultaneous multiphoton scattering from a single emitter. In contrast, the total reflected field—comprising the reflected driving field and incoherent scattering—displays perfect antibunching, arising from quantum interference that cancels two-photon probability amplitudes. By spectrally filtering the reflected field, we tune the relative contributions of coherent and incoherent components, observing transitions in photon statistics from antibunching to superbunching, or to Poissonian light. Supported by master-equation simulations and an interference-based model, these results uncover the hidden but fundamental role of multiphoton dynamics in resonance fluorescence, and open avenues for generating nonclassical light in cavity and waveguide quantum electrodynamics.
Controlling the photon statistics of light is paramount for quantum science and technologies. Recently, we demonstrated that transmitting resonant laser light past an ensemble of two-level emitters can result in a stream of single photons or excess photon pairs. This transformation is due to quantum interference between the transmitted laser light and the incoherently scattered photon pairs [Prasad et al., Nat. Photonics 14, 719 (2020)NPAHBY1749-488510.1038/s41566-020-0692-z]. Here, using the dispersion of the atomic medium, we actively control the relative quantum phase between these two components. We thereby realize a tunable two-photon interferometer and observe interference fringes in the normalized photon coincidence rate. When tuning the relative phase, the coincidence rate varies periodically, giving rise to a continuous modification of the photon statistics from antibunching to bunching. Beyond the fundamental insight that there exists a tunable quantum phase between incoherent and coherent light that dictates the photon statistics, our results lend themselves to the development of novel quantum light sources.
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 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.
Laser light possesses perfect coherence, but cannot be attenuated to single photons via linear optics. An elegant route to convert laser light into single photons is based on photon blockade in a cavity with a single atom in the strong coupling regime. However, the single-photon purity achieved by this method remains relatively low. Here we propose an interference-based approach where laser light can be transformed into single photons by destructively interfering with a weak but super-bunched incoherent field emitted from a cavity coupling to a single quantum emitter. We demonstrate this idea by measuring the reflected light of a laser field which drives a double-sided optical microcavity containing a single artificial atom-quantum dot (QD) in the Purcell regime. The reflected light consists of a superposition of the driving field with the cavity output field. We achieve the second-order autocorrelation g2(0)=0.030+-0.002 and the two-photon interference visibility 94.3%+-0.2. By separating the coherent and incoherent fields in the reflected light, we observe that the incoherent field from the cavity exhibits super-bunching with g2(0)=41+-2 while the coherent field remains Poissonian statistics. By controlling the relative amplitude of coherent and incoherent fields, we verify that photon statistics of reflected light is tuneable from perfect anti-bunching to super-bunching in agreement with our predictions. Our results demonstrate photon statistics of light as a quantum interference phenomenon that a single QD can scatter two photons simultaneously at low driving fields in contrast to the common picture that a single two-level quantum emitter can only scatter (or absorb and emit) single photons. This work opens the door to tailoring photon statistics of laser light via cavity or waveguide quantum electrodynamics and interference.