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arXiv:2209.05786 · Nano Letters

Superradiant Electron Energy Loss Spectroscopy

Ron Ruimy, Alexey A. Gorlach, Gefen Baranes, Ido E. Kaminer

Published Jan 23, 2023• 8 citations
arXivHTMLPDF

Abstract

We analyze the interaction between a free electron and an ensemble of identical optical emitters. The mutual coherence and correlations between the emitters can enhance the interaction with each electron and become imprinted on its energy spectrum. We present schemes by which such collective interactions can be realized. As a possible application, we investigate free-electron interactions with superradiant systems, showing how electrons can probe the ultrafast population dynamics of superradiance.

DOI
10.1021/acs.nanolett.2c03396

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We analyze the interaction between a free electron and an ensemble of identical optical emitters. The mutual coherence and correlations between the emitters can enhance the interaction with each electron and become imprinted on its energy spectrum. We present schemes by which such collective interactions can be realized. As a possible application, we investigate free-electron interactions with superradiant systems, showing how electrons can probe the ultrafast population dynamics of superradiance.
Recent advances in time-resolved cathodoluminescence have enabled ultrafast studies of single emitters in quantum materials with femtosecond temporal resolution. Here, we develop a quantum theory modeling the dynamics of free electrons interacting with quantum emitters in arbitrary initial states. Our analysis reveals that a free electron can induce transient coherent oscillations in the populations when the system is initially prepared in a coherent superposition of its states. Moreover, the electron energy spectrum exhibits a clear signature of the quantum coherence and sensitivity to the transition frequency of the emitter. These coherence effects manifest themselves as oscillations in the zero-loss peak of the spectral energy-loss probability. Our findings pave the way for characterization of quantum-coherent dynamics of individual quantum emitters by electron-probes.
There exist two families of superradiance phenomena: relying on free electrons or on correlated emission by ensembles of atoms. Here we investigate emission from ensembles of atoms driven by coherently shaped free electrons. This interaction creates superradiance emerging from both the atoms' and the electrons' coherence---with emission intensity that scales quadratically in both the number of atoms and number of electrons. This phenomenon enables electrons to become probes of quantum correlations in matter, with high temporal and spatial resolution.
When multiple quantum emitters radiate, their emission rate may be enhanced or suppressed due to collective interference in a process known as super- or subradiance. Such processes are well known to occur also in light emission from free electrons, known as coherent cathodoluminescence. Unlike atomic systems, free electrons have an unbounded energy spectrum, and, thus, all their emission mechanisms rely on electron recoil, in addition to the classical properties of the dielectric medium. To date, all experimental and theoretical studies of super- and subradiance from free electrons assumed only classical correlations between particles. However, dependence on quantum correlations, such as entanglement between free electrons, has not been studied. Recent advances in coherent shaping of free-electron wave functions motivate the investigation of such quantum regimes of super- and subradiance. In this Letter, we show how a pair of coincident path-entangled electrons can demonstrate either super- or subradiant light emission, depending on the two-particle wave function. By choosing different free-electron Bell states, the spectrum and emission pattern of the light can be reshaped, in a manner that cannot be accounted for by a classical mixed state. We show these results for light emission in any optical medium and discuss their generalization to many-body quantum states. Our findings suggest that light emission can be sensitive to the explicit quantum state of the emitting matter wave and possibly serve as a nondestructive measurement scheme for measuring the quantum state of many-body systems.
Quantum cooperativity is evident in light-matter platforms where quantum emitter ensembles are interfaced with confined optical modes and are coupled via the ubiquitous electromagnetic quantum vacuum. Cooperative aspects such as dipole-dipole interactions and subradiance find applications in the design of nanoscale coherent light sources and highly-reflective quantum metasurfaces made up of hundreds of optically trapped atoms, in the implementation of topological quantum optics on subwavelength arrays of emitters, in quantum metrology and quantum information. The quick bursts of radiation from a collection of quasi-indistiguishable emitters provides an alternative approach to standard lasers by introducing superradiant lasers operating at extremely low intracavity power. This tutorial provides a set of theoretical tools to tackle the behavior responsible for the onset of cooperativity in light-matter systems by extending open quantum system dynamics methods, such as the master equation and quantum Langevin equations, to electron-photon interactions in strongly coupled and correlated quantum emitters ensembles. These analytical approaches are then also extended to frequency disordered or vibronically coupled quantum emitter ensembles with wide relevance ranging from atoms in optical lattices, quantum dots in solid state environments or molecular quantum systems.
Superradiance is a quantum phenomenon in which coherence between emitters results in enhanced and directional radiative emission. Many quantum optical phenomena can be characterized by the two-time quantum correlation function g(2)(t,τ)g^{(2)}(t,τ)g(2)(t,τ), which describes the photon statistics of emitted radiation. However, the critical task of determining g(2)(t,τ)g^{(2)}(t,τ)g(2)(t,τ) becomes intractable for large emitter ensembles due to the exponential scaling of the Hilbert space dimension with the number of emitters. Here, we analyse and benchmark two approximate numerical sampling methods applicable to emitter arrays embedded within electromagnetic environments, which generally provide upper and lower bounds for g(2)(t,0)g^{(2)}(t,0)g(2)(t,0). We also introduce corrections to these methods (termed offset corrections) that significantly improve the quality of the predictions. The optimal choice of method depends on the total number of emitters, such that taken together, the two approaches provide accurate descriptions across a broad range of important regimes. This work therefore provides new theoretical tools for studying the well-known yet complex phenomenon of superradiance in large ensembles of quantum emitters.
The interaction between light and matter has captivated physicists for centuries, from early studies of vision and refraction in ancient Greece to the development of quantum mechanics and quantum electrodynamics in the past century. While the response of a single quantum emitter to light is well understood, the radiative properties of an ensemble of closely spaced emitters are far more intricate. Coupling to a shared electromagnetic environment induces coherent and dissipative interactions between emitters, giving rise to a collective response that cannot be captured by treating them independently. In the regime of few excitations, the system hosts delocalized subradiant states, that is, coherent superpositions that are largely decoupled from the electromagnetic field and thus decay at suppressed rates. While this weak coupling makes subradiant states attractive for quantum technologies, it also renders them difficult to manipulate. At higher excitation densities, the intrinsic nonlinearity of emitters and the exponential growth of the Hilbert space make theoretical and numerical descriptions of the system and its dynamics increasingly challenging. This thesis explores two fundamental questions: How can subradiant and dark states be selectively accessed and harnessed for practical applications in quantum technologies? And how can interacting ensembles of quantum emitters be efficiently simulated to uncover their many-body physics? The first part of the thesis develops protocols for controlling and addressing dark states in free-space and waveguide-coupled atomic arrays, demonstrating their utility in quantum storage and the deterministic generation of entangled photonic states. Incorporating atomic motion, we further show that collective subradiant states can enhance cooling in dense atomic arrays, offering new avenues for controlling motional dynamics. In the second part, we introduce cumulant expansions of the equations of motion as a powerful tool to analytically and numerically investigate collective decay in the many-body regime. We first examine the collective decay of fully excited atomic arrays in free space, characterizing the onset and scaling of the superradiant burst across different geometries. In collaboration with experiments on ultracold erbium atoms in optical lattices, we provide the first direct observations of many-body collective effects in free-space ordered arrays, including early-time superradiant bursts, late-time subradiant tails, and the emergence of atomic correlations throughout the dynamics. Finally, we theoretically and numerically explore the transient formation of multi-excitation subradiant states, and demonstrate how the existence of multiple dissipation channels suppresses steady-state superradiance in extended arrays.