Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

arXiv:1710.06483 · Physical review. B./Physical review. B

Colossal photon bunching in quasiparticle-mediated nanodiamond cathodoluminescence

Matthew A. Feldman, Eugene Dumitrescu, Denzel Bridges, Matthew F. Chisholm, Roderick B. Davidson, Philip G. Evans, Jordan A. Hachtel, Anming Hu, Raphael C. Pooser, Richard F. Haglund, Benjamin J. Lawrie

Published Feb 15, 2018• 35 citations
arXivHTMLPDF

Abstract

Nanoscale control over the second-order photon correlation function ${g}^{(2)}(\ensuremath{\tau})$ is critical to emerging research in nonlinear nanophotonics and integrated quantum information science. Here we report on quasiparticle control of photon bunching with ${g}^{(2)}(0)>45$ in the cathodoluminescence of nanodiamond nitrogen vacancy (${\mathrm{NV}}^{0}$) centers excited by a converged electron beam in an aberration-corrected scanning transmission electron microscope. Plasmon-mediated ${\mathrm{NV}}^{0}$ cathodoluminescence exhibits a 16-fold increase in luminescence intensity correlated with a threefold reduction in photon bunching compared with that of uncoupled ${\mathrm{NV}}^{0}$ centers. This effect is ascribed to the excitation of single temporally uncorrelated ${\mathrm{NV}}^{0}$ centers by single surface plasmon polaritons. Spectrally resolved Hanbury Brown--Twiss interferometry is employed to demonstrate that the bunching is mediated by the ${\mathrm{NV}}^{0}$ phonon sidebands, while no observable bunching is detected at the zero-phonon line. The data are consistent with fast phonon-mediated recombination dynamics, a conclusion substantiated by agreement between Bayesian regression and Monte Carlo models of superthermal ${\mathrm{NV}}^{0}$ luminescence.

DOI
10.1103/physrevb.97.081404

Related papers

Purcell effect of nitrogen-vacancy centers in nanodiamond coupled to propagating and localized surface plasmons revealed by photon-correlation cathodoluminescence

Sotatsu Yanagimoto, Naoki Yamamoto, Takumi Sannomiya +1 more

We measured the second-order correlation function of the cathodoluminescence intensity and investigated the Purcell effect by comparing the lifetimes of quantum emitters with and without metal structure. The increase in the electromagnetic local density of state due to the coupling of a quantum emitter with a plasmonic structure causes a shortening of the emitter lifetime. Since the plasmon-enhanced electric field is confined well below the wavelength of light, the quantum emitter lifetime is changed in the nanoscale range. In this study, we combined cathodoluminescence in scanning (transmission) electron microscopy with Hanbury Brown--Twiss interferometry to measure the Purcell effect with nanometer and nanosecond resolutions. We used nitrogen-vacancy centers contained in nanodiamonds as the emitters and compared their lifetime in different environments: on a thin $\mathrm{Si}{\mathrm{O}}_{2}$ membrane, on a thick flat silver film, and embedded in a silver film. The lifetime reductions of nitrogen-vacancy centers were observed in the samples with silver. We evaluated the lifetime by analytical calculation and numerical simulations and revealed the Purcell effects of emitters coupled to the propagating and localized surface plasmons.

arXiv:2012.11224•Physical review. B./Physical review. B•May 14, 2021•31 citations

Colossal Bunching in Nanodiamond Cathodoluminescence

Matthew A. Feldman, Roderick B. Davidson, Jordan A. Hachtel +7 more

Photon bunching with g(2)(0)>30 was observed in cathodoluminescence from nanodiamond particles evanescently coupled to Ag surface-plasmon polaritons. Comparisons with the photon bunching of isolated diamond nanoparticles point to Ag-plasmon-mediated decoherence processes.

Frontiers in Optics•Jan 1, 2017•0 citations

Spatially Resolved Quantum Nano-Optics of Single Photons Using an Electron Microscope

Luiz H. G. Tizei, Mathieu Kociak

We report on the experimental demonstration of single-photon state generation and characterization in an electron microscope. In this aim we have used low intensity relativistic (energy between 60 and 100 keV) electrons beams focused in a ca. 1 nm probe to excite diamond nanoparticles. This triggered individual neutral nitrogen-vacancy centers to emit photons which could be gathered and sent to a Hanbury Brown-Twiss intensity interferometer. The detection of a dip in the correlation function at small time delays clearly demonstrates antibunching and thus the creation of nonclassical light states. Specifically, we have also demonstrated single-photon states detection. We unveil the mechanism behind quantum states generation in an electron microscope, and show that it clearly makes cathodoluminescence the nanometer scale analog of photoluminescence. By using an extremely small electron probe size and the ability to monitor its position with subnanometer resolution, we also show the possibility of measuring the quantum character of the emitted beam with deep subwavelength resolution.

arXiv:1301.0922•Physical Review Letters•Apr 9, 2013•117 citations

Spatially and spectrally resolved cathodoluminescence with fast electrons: A tool for background subtraction in luminescence intensity second‐order correlation measurements applied to subwavelength inhomogeneous diamond nanocrystals

Luiz H. G. Tizei, Sophie Meuret, Sounderya Nagarajan +4 more

Measurements of the photon second‐order correlation function, g (2) ( τ ), is a common tool for the characterization of single photon emitters, like nitrogen‐vacancy color centers in diamond. Such measurement requires background photoluminescence correction, which is easy when this background is homogeneous on a few wavelengths scale. However, if the sample contains emitting centers separated by a distance smaller than the optical diffraction limit, and having different and overlapping emission, these background correction techniques cannot be applied. We have recently shown that cathodoluminescence (CL) can be used to measure g (2) ( τ ) at the subwavelength scale. Here we propose a method, based on spatially and spectrally resolved CL, to subtract the background taking into account the nanometer spatial distribution of the emitted light. To this end, a nanometer‐resolved spectrum image is acquired on the same region where the g (2) ( τ ) is measured. As an example, we show the use of this method to the subtraction of the H3 background signal from a g (2) ( τ ) measurement done on NV 0 color centers.

physica status solidi (a)•Jul 30, 2013•19 citations

Nanodiamond grain boundaries and lattice expansion drive Silicon vacancy emission heterogeneity

Daniel K. Angell, Shuo Li, Hendrik Utzat +8 more

Silicon-vacancy (SiV$^-$) centers in diamond are promising candidates as sources of single-photons in quantum networks due to their minimal phonon coupling and narrow optical linewidths. Correlating SiV$^-$ emission with the defect's atomic-scale structure is important for controlling and optimizing quantum emission, but remains an outstanding challenge. Here, we use cathodoluminescence imaging in a scanning transmission electron microscope (STEM) to elucidate the structural sources of non-ideality in the SiV$^-$ emission from nanodiamonds with sub-nanometer-scale resolution. We show that different crystalline domains of a nanodiamond exhibit distinct zero-phonon line (ZPL) energies and differences in brightness, while near-surface SiV$^-$ emitters remain bright. We correlate these changes with local lattice expansion using 4D STEM and diffraction, and show that associated blue shifts from the ZPL are due to defect density heterogeneity, while red shifts are due to lattice distortions.

arXiv:2202.07879•Feb 16, 2022•0 citations

Sub‐to‐super‐Poissonian photon statistics in cathodoluminescence of color center ensembles in isolated diamond crystals

Saskia Fiedler, Sergii Morozov, Danylo Komisar +8 more

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.

arXiv:2302.03386•Nanophotonics•May 26, 2023•15 citations
Nanoscale control over the second-order photon correlation function g(2)(\ensuremathτ){g}^{(2)}(\ensuremath{\tau})g(2)(\ensuremathτ) is critical to emerging research in nonlinear nanophotonics and integrated quantum information science. Here we report on quasiparticle control of photon bunching with g(2)(0)>45{g}^{(2)}(0)>45g(2)(0)>45 in the cathodoluminescence of nanodiamond nitrogen vacancy (NV0{\mathrm{NV}}^{0}NV0) centers excited by a converged electron beam in an aberration-corrected scanning transmission electron microscope. Plasmon-mediated NV0{\mathrm{NV}}^{0}NV0 cathodoluminescence exhibits a 16-fold increase in luminescence intensity correlated with a threefold reduction in photon bunching compared with that of uncoupled NV0{\mathrm{NV}}^{0}NV0 centers. This effect is ascribed to the excitation of single temporally uncorrelated NV0{\mathrm{NV}}^{0}NV0 centers by single surface plasmon polaritons. Spectrally resolved Hanbury Brown--Twiss interferometry is employed to demonstrate that the bunching is mediated by the NV0{\mathrm{NV}}^{0}NV0 phonon sidebands, while no observable bunching is detected at the zero-phonon line. The data are consistent with fast phonon-mediated recombination dynamics, a conclusion substantiated by agreement between Bayesian regression and Monte Carlo models of superthermal NV0{\mathrm{NV}}^{0}NV0 luminescence.
We measured the second-order correlation function of the cathodoluminescence intensity and investigated the Purcell effect by comparing the lifetimes of quantum emitters with and without metal structure. The increase in the electromagnetic local density of state due to the coupling of a quantum emitter with a plasmonic structure causes a shortening of the emitter lifetime. Since the plasmon-enhanced electric field is confined well below the wavelength of light, the quantum emitter lifetime is changed in the nanoscale range. In this study, we combined cathodoluminescence in scanning (transmission) electron microscopy with Hanbury Brown--Twiss interferometry to measure the Purcell effect with nanometer and nanosecond resolutions. We used nitrogen-vacancy centers contained in nanodiamonds as the emitters and compared their lifetime in different environments: on a thin SiO2\mathrm{Si}{\mathrm{O}}_{2}SiO2​ membrane, on a thick flat silver film, and embedded in a silver film. The lifetime reductions of nitrogen-vacancy centers were observed in the samples with silver. We evaluated the lifetime by analytical calculation and numerical simulations and revealed the Purcell effects of emitters coupled to the propagating and localized surface plasmons.
We report on the experimental demonstration of single-photon state generation and characterization in an electron microscope. In this aim we have used low intensity relativistic (energy between 60 and 100 keV) electrons beams focused in a ca. 1 nm probe to excite diamond nanoparticles. This triggered individual neutral nitrogen-vacancy centers to emit photons which could be gathered and sent to a Hanbury Brown-Twiss intensity interferometer. The detection of a dip in the correlation function at small time delays clearly demonstrates antibunching and thus the creation of nonclassical light states. Specifically, we have also demonstrated single-photon states detection. We unveil the mechanism behind quantum states generation in an electron microscope, and show that it clearly makes cathodoluminescence the nanometer scale analog of photoluminescence. By using an extremely small electron probe size and the ability to monitor its position with subnanometer resolution, we also show the possibility of measuring the quantum character of the emitted beam with deep subwavelength resolution.
Measurements of the photon second‐order correlation function, g (2) ( τ ), is a common tool for the characterization of single photon emitters, like nitrogen‐vacancy color centers in diamond. Such measurement requires background photoluminescence correction, which is easy when this background is homogeneous on a few wavelengths scale. However, if the sample contains emitting centers separated by a distance smaller than the optical diffraction limit, and having different and overlapping emission, these background correction techniques cannot be applied. We have recently shown that cathodoluminescence (CL) can be used to measure g (2) ( τ ) at the subwavelength scale. Here we propose a method, based on spatially and spectrally resolved CL, to subtract the background taking into account the nanometer spatial distribution of the emitted light. To this end, a nanometer‐resolved spectrum image is acquired on the same region where the g (2) ( τ ) is measured. As an example, we show the use of this method to the subtraction of the H3 background signal from a g (2) ( τ ) measurement done on NV 0 color centers.
Silicon-vacancy (SiV−^-−) centers in diamond are promising candidates as sources of single-photons in quantum networks due to their minimal phonon coupling and narrow optical linewidths. Correlating SiV−^-− emission with the defect's atomic-scale structure is important for controlling and optimizing quantum emission, but remains an outstanding challenge. Here, we use cathodoluminescence imaging in a scanning transmission electron microscope (STEM) to elucidate the structural sources of non-ideality in the SiV−^-− emission from nanodiamonds with sub-nanometer-scale resolution. We show that different crystalline domains of a nanodiamond exhibit distinct zero-phonon line (ZPL) energies and differences in brightness, while near-surface SiV−^-− emitters remain bright. We correlate these changes with local lattice expansion using 4D STEM and diffraction, and show that associated blue shifts from the ZPL are due to defect density heterogeneity, while red shifts are due to lattice distortions.
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.