Abstract Cathodoluminescence (CL), the emission of light induced by accelerated free electrons, has been extensively utilized in various applications, such as displays, streak cameras, and high-spatial-resolution analysis of optical materials, surpassing the diffraction limit of light. Despite its long history, the photon statistics of CL have only recently been examined, revealing unexpectedly large bunching of photons. Here we find that this peculiar photon bunching contains information of intervening excitation processes before the photon emission, which can be extracted from the photon statistics within each excitation event by a single free electron. Using this approach, we experimentally unveiled the statistical differences of coherent CL involving a single electromagnetic interaction process and incoherent CL involving multiple excitation processes. The developed formulation is universally applicable for particle generation processes in general to investigate the nature of cascade reactions.
Abstract Cathodoluminescence (CL), the emission of light induced by accelerated free electrons, has been extensively utilized in various applications, such as displays, streak cameras, and high-spatial-resolution analysis of optical materials, surpassing the diffraction limit of light. Despite its long history, the photon statistics of CL have only recently been examined, revealing unexpectedly large bunching of photons. Here we find that this peculiar photon bunching contains information of intervening excitation processes before the photon emission, which can be extracted from the photon statistics within each excitation event by a single free electron. Using this approach, we experimentally unveiled the statistical differences of coherent CL involving a single electromagnetic interaction process and incoherent CL involving multiple excitation processes. The developed formulation is universally applicable for particle generation processes in general to investigate the nature of cascade reactions.
Electron--photon quantum entanglement in an electron microscope paves the way for a new quantum platform, enabling the integration of quantum functionalities into electron microscopy and opening opportunities for quantum imaging and quantum sensing at the nanoscale. To realize such a platform, it is crucial to understand the degree and nature of electron--photon entanglement in cathodoluminescence (CL). However, its dependence on electron-beam properties, particularly transverse coherence, remains unclear. Here, we present a theoretical framework describing the quantum state of an electron--photon pair generated in coherent CL from a system with translational invariance in the plane perpendicular to the electron beam, as can be realized, for example, in transition radiation at a planar interface. By expressing the scattered state directly in terms of the luminescence spectrum, we evaluate the entanglement using both subsystem purity and an Einstein--Podolsky--Rosen-type criterion. These two measures enable a clear distinction among wave-like, particle-like, and classical regimes in terms of spatial and momentum entanglement in the electron--photon system. Our analysis identifies the roles of the electron's transverse and longitudinal coherence, as well as the photon's spectral width, and reveals the conditions under which strong spatial entanglement emerges. This unified perspective clarifies the nature of electron--photon quantum correlations in coherent CL and advances the development of quantum-enabled functionalities in electron microscopy.
We propose a theoretical model of a master equation for cathodoluminescence (CL). The master equation describes simultaneous excitation of multiple emitters by an incoming electron and radiative decay of individual emitters. We investigate the normalized second-order correlation function, ${g}^{(2)}(\ensuremath{\tau})$, of this model. We derive the exact formula for the zero-time delay correlation, g(2)(0), and show that the model successfully describes giant bunching (superbunching) in the CL. We also derive an approximate form of ${g}^{(2)}(\ensuremath{\tau})$, which is valid for small excitation rate. Furthermore, we discuss the state of the radiation field of the CL. We reveal that the superbunching results from a mixture of an excited photon state and the vacuum state and that this type of state is realized in the CL.
Abstract Impurity‐vacancy centers in diamond offer a new class of robust photon sources with versatile quantum properties. While individual color centers commonly act as single‐photon sources, their ensembles have been theoretically predicted to have tunable photon‐emission statistics. Importantly, the particular type of excitation affects the emission properties of a color center ensemble within a diamond crystal. While optical excitation favors non‐synchronized excitation of color centers within an ensemble, electron‐beam excitation can synchronize the emitters excitation and thereby provides a control of the second‐order correlation function g 2 (0). In this letter, we demonstrate experimentally that the photon stream from an ensemble of color centers can exhibit g 2 (0) both above and below unity, thereby confirming long standing theoretical predictions by Meuret et al. [S. Meuret, L. H. G. Tizei, T. Cazimajou, et al., “Photon bunching in cathodoluminescence,” Phys. Rev. Lett. , vol. 114, no. 19, p. 197401, 2015.]. Such a photon source based on an ensemble of few color centers in a diamond crystal provides a highly tunable platform for informational technologies operating at room temperature.
Since the introduction of time-resolved direct electron detectors to transmission electron microscopy (TEM), there has been a growing interest in studying the correlations between an electron and the cathodoluminescence (CL) photons it produces [1,2,3]. Recent studies using coincidence measurements in both continuous [4] and discrete variables [5] have shown correlations that exceed the classical limits for separable states, thus demonstrating quantum entanglement between free electrons and photons. We present our continuous-variable approach [4], showing how ghost imaging [6], a method adapted from photonic quantum optics, can be used to demonstrate entanglement and even EPR-like behaviour of the joint electron- photon state. For this purpose, we generate correlated electron-photon pairs via transition radiation from 200 keV electrons passing a 50 nm monocrystalline silicon membrane. We detect the CL photons in a time-resolved manner, using a custom parabolic mirror and a single-photon counter. Employing a Timepix3 based direct electron detector we are able to determine which photons arrive in time with a corresponding electron. These electron-photon pairs exhibit precise (anti-)correlations in momentum and position. Placing a known absorptive mask in the photon beam path while measuring the electron in imaging and diffraction mode allows us to extract the joint position and momentum uncertainties of the electron–photon pair. We use these measurements to evaluate entanglement criteria such as the MGTV inequality [7] and the Reid- EPR bound [8]. We hope that these results will help to make entanglement available as a resource for electron microscopy, enabling novel measurement schemes inspired by photonic quantum optics.
Quantum optics performed at the nanometer scale is an important challenge, especially for quantum emitters characterization. They can be point defects in material (few ang- ströms) or confined structures of a few nanometers. A way to reach this scale is by using cathodoluminescence (CL) performed in a scanning transmission electron microscope (CL- STEM), which has only recently been done [1]. However, when aiming at studying the statistical properties of the light coming out of a CL experiment, which is necessary to e. g. study the quantum nature of Single Photon Emitters (SPE) emission, dedicated expe- riments on top of regular CL ones have to be designed. Few months before my arrival in the STEM-group of the LPS, an intensity interferometry experiment (HBT) that measures the autocorrelation function g(2) of the CL signal intensity was built [2]. It is well known that the clear signature of SPE as measured in photoluminescence (PL) is antibunching in the g(2)(τ), namely that the autocorrelation function is always less than one. It was re- cently demonstrated on a famous SPE, the Nitrogen vacancy (NV) defect in diamond, that CL-STEM is similar to PL when only one SPE is involved. In this thesis we will see how CL-STEM allowed to characterize a new point defect in h-BN, showing the relevance of HBT experiments in a CL-STEM for discovering and characterizing new SPE. However, by studying the excitation of multiple SPE in CL, we discovered a new emission phenomenon, characterized by a huge bunching effect of the g(2)(τ) function (g(2)(0) > 35), in complete contradiction to PL measurements and expectations (g(2)(0)<1). In my thesis manuscript, this surprising effect will be experimentally investigated, theoretically explained and applied to lifetime measurement at the nanometer scale. Because quantum optics is often linked to quantum plasmonics, I will present, to conclude, a theoretical proposal, in collaboration with J. Garcia de Abajo, about quantum plasmonics measurement in a STEM.
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