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, 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 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.
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.
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.
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.
Introduction Quantum optics provides a complete description of the resonant interaction of light and a material system. The light scattered as a result of this interaction – the resonance fluorescence – provides a means to monitor and affect the material system's dynamics and also allows for the generation of nonclassical states of the electromagnetic field. Initial theoretical studies characterizing resonance fluorescence addressed fundamental questions regarding the necessity of quantizing the electromagnetic field. This is a particularly illustrative period in optical physics where multiple theories existed that might describe resonance fluorescence – semi-classical optical Bloch equations [1, 2] or quantum electrodynamics [4, 3] – and experimental evidence was necessary to identify the appropriate theoretical framework. Indeed, experiments in 1974 and 1977 investigating the resonance fluorescence lineshape [5, 6] and the photon statistics of the scattered light [7] vindicated the full quantum electrodynamical description of light-matter interaction over other models. In the subsequent 30 years, resonance fluorescence has been used as a high-resolution spectroscopic probe of a variety of physical systems, as a means to investigate quantum coherence in atomic gases and, with the current interest in quantum information science (QIS), as a tool for quantum-state preparation, measurement and control in trapped ions [8]. During this same time period, advances in material science have ushered in an era where it is possible to grow and fabricate solid-state devices at length scales commensurate with the quantum confinement of electrons and holes. It is only recently that resonance fluorescence has been observed from the prototypical artificial nanostructure exhibiting three-dimensional quantum confinement – a single semiconductor quantum dot (QD) [9].
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.