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Photon bunching in incoherent cathodoluminescence (CL) spectroscopy originates from the fact that a single high-energy electron can generate multiple photons when interacting with a material, thus, revealing key properties of electron-matter excitation. Contrary to previous works based on Monte Carlo modeling, here we present a fully analytical model describing the amplitude and shape of the second order autocorrelation function ( g (2) (τ)) for continuous and pulsed electron beams. Moreover, we extend the analysis of photon bunching to ultrashort electron pulses, in which up to 500 electrons per pulse excite the sample within a few picoseconds. We obtain a simple equation relating the bunching strength ( g (2) (0)) to the electron beam current, emitter decay lifetime, pulse duration, in the case of pulsed electron beams, and electron excitation efficiency (γ), defined as the probability that an electron creates at least one interaction with the emitter. The analytical model shows good agreement with the experimental data obtained on InGaN/GaN quantum wells using continuous, ns-pulsed (using beam blanker) and ultrashort ps-pulsed (using photoemission) electron beams. We extract excitation efficiencies of 0.13 and 0.05 for 10 and 8 keV electron beams, respectively, and we observe that nonlinear effects play no compelling role, even after excitation with ultrashort and dense electron cascades in the quantum wells., Competing Interests: The authors declare the following competing financial interest(s): T.C. is an employee and A.P. is the co-founder and co-owner of Delmic BV, a company that produces the cathodoluminescence system that was used in this work., (© 2021 The Authors. Published by American Chemical Society.)

Nitrogen-vacancy (NV) centers in diamond are reliable single-photon emitters, with applications in quantum technologies and metrology. Two charge states are known for NV centers, NV 0 and NV - , with the latter being mostly studied due to its long electron spin coherence time. Therefore, control over the charge state of the NV centers is essential. However, an understanding of the dynamics between the different states still remains challenging. Here, conversion from NV - to NV 0 due to electron-induced carrier generation is shown. Ultrafast pump-probe cathodoluminescence spectroscopy is presented for the first time, with electron pulses as pump and laser pulses as probe, to prepare and read out the NV states. The experimental data are explained with a model considering carrier dynamics (0.8 ns), NV 0 spontaneous emission (20 ns), and NV 0 → NV - back transfer (500 ms). The results provide new insights into the NV - → NV 0 conversion dynamics and into the use of pump-probe cathodoluminescence as a nanoscale NV characterization tool., Competing Interests: The authors declare no competing financial interest., (Copyright © 2019 American Chemical Society.)

We investigate the nanoscale excitation of Ag nanocubes with coherent cathodoluminescence imaging spectroscopy (CL) to resolve the factors that determine the spatial resolution of CL as a deep-subwavelength imaging technique. The 10-30 keV electron beam coherently excites localized plasmons in 70 nm Ag cubes at 2.4 and 3.1 eV. The radiation from these plasmon modes is collected in the far-field together with the secondary electron intensity. CL line scans across the nanocubes show exponentially decaying tails away from the cube that reveal the evanescent coupling of the electron field to the resonant plasmon modes. The measured CL decay lengths range from 8 nm (10 keV) to 12 nm (30 keV) and differ from the calculated ones by only 1-3 nm. A statistical model of electron scattering inside the Ag nanocubes is developed to analyze the secondary electron images and compare them with the CL data. The Ag nanocube edges are derived from the CL line scans with a systematic error less than 3 nm. The data demonstrate that CL probes the electron-induced plasmon fields with nanometer accuracy., Competing Interests: The authors declare the following competing financial interest(s): A.P. is co-founder and co-owner and T.C. is employee of Delmic BV, a company that produces the cathodoluminescence system that was used in this work.