Skip to content

Colossal photon bunching in quasiparticle-mediated nanodiamond cathodoluminescence

MetadataDetails
Publication Date2018-02-15
JournalPhysical review. B./Physical review. B
AuthorsMatthew Feldman, Eugene Dumitrescu, Denzel Bridges, Matthew F. Chisholm, Roderick B. Davidson
InstitutionsUniversity of Tennessee at Knoxville, Vanderbilt University
Citations34
AnalysisFull AI Review Included

Technical Documentation & Analysis: Colossal Photon Bunching in Nanodiamond CL

Section titled “Technical Documentation & Analysis: Colossal Photon Bunching in Nanodiamond CL”

This document analyzes the research paper “Colossal photon bunching in quasiparticle-mediated nanodiamond cathodoluminescence” (arXiv:1710.06483v2) to provide technical specifications and align the material requirements with 6CCVD’s advanced MPCVD diamond capabilities.


This research demonstrates unprecedented control over photon statistics in nanodiamond Nitrogen Vacancy (NV0) centers, achieving colossal photon bunching critical for quantum information science.

  • Record Bunching: Observation of maximum second-order photon correlation function g(2)(0) = 49.0, an order of magnitude greater than previous room-temperature reports.
  • Spectral Dependence: Bunching is exclusively mediated by the NV0 phonon sideband (PSB), confirming faster phonon-mediated recombination dynamics. Negligible bunching was detected at the Zero-Phonon Line (ZPL).
  • Excitation Method: Cathodoluminescence (CL) driven by a 60-keV electron beam in an aberration-corrected Scanning Transmission Electron Microscope (STEM) was used to achieve nanoscale spatial resolution.
  • Plasmonic Interaction: Coupling nanodiamonds to a single-crystal Ag nanoplate resulted in a 16-fold increase in CL intensity, attributed to SPP-NV center scattering, but correlated with a 3-fold reduction in photon bunching.
  • Modeling Validation: A phenomenological Monte Carlo model successfully reproduced the monotonic decrease of g(2)(0) with increasing electron beam current and validated the spectral distribution of bunching.
  • Future Impact: The ability to control g(2)(τ) via quasiparticle interactions provides a critical tool for developing high-efficiency nonlinear nanophotonics and steady-state quantum entanglement schemes.

The following hard data points were extracted from the experimental results:

ParameterValueUnitContext
Maximum Photon Bunching (g(2)(0))49.0 (± 0.9)DimensionlessMaximum observed value across 66 measurements.
Mean Fitted Lifetime (τeff)21.1 (± 0.9)nsLifetime of NV0 centers in nanodiamonds.
Electron Beam Energy60keVOperating energy of the VG601 STEM.
Electron Beam Current Range0.2 - 2.1nARange used for g(2)(τ) statistics.
CL Intensity Enhancement (Plasmonic)16foldAg-NV hybrid vs. uncoupled NV ensemble (at 0.6 nA).
Bunching Reduction (Plasmonic)3foldCorrelated with 16-fold intensity increase.
Nanodiamond Diameter120nmContaining approximately 1200 NV0 centers per particle.
Silver Nanoplate Thickness100nmSubstrate used for plasmonic coupling.
NV0 Zero-Phonon Line (ZPL)575nmWavelength used for ZPL filtering (5 nm bandwidth).
Phonon Sideband (PSB) Filter610nmLong-pass filter (LP610) used to isolate PSB emission.

The experiment relied on precise material integration and advanced electron microscopy techniques to achieve spectrally and spatially resolved photon correlation measurements.

  1. Material Preparation: Nanodiamonds (120 nm diameter, containing ~1200 NV0 centers) were dropcast onto a single-crystal silver nanoplate (100 nm thick, 100 ”m wide).
  2. Excitation System: An aberration-corrected VG601 STEM was utilized, operating at room temperature with an electron energy of 60-keV.
  3. CL Collection Setup: A 2-sr Aluminum parabolic mirror, integrated into the STEM, collected the collimated cathodoluminescence (CL).
  4. Correlation Measurement: The CL was analyzed using a Hanbury Brown-Twiss (HB-T) interferometer setup, employing two single-photon counting modules (SPCMs) and a HydraHarp 400 time-interval analyzer (256 ps bin sizes).
  5. Spectral Isolation:
    • The NV0 ZPL was isolated using a 575-nm bandpass filter (5 nm bandwidth).
    • The phonon sideband (PSB) was isolated using a 610-nm long-pass filter (LP610).
  6. Data Analysis: The second-order correlation function g(2)(τ) was calculated and analyzed using self-consistent Bayesian regression and compared against a phenomenological Monte Carlo model incorporating multiple radiative transitions.

The reported research highlights the critical need for high-quality diamond materials and precise integration capabilities to advance quantum nanophotonics. 6CCVD is uniquely positioned to supply the next generation of custom diamond substrates required to replicate and extend this work, particularly in optimizing Purcell factors and controlling quasiparticle interactions.

Research Requirement/Challenge6CCVD Solution & CapabilityTechnical Advantage for Quantum Research
High-Purity Diamond HostOptical Grade Single Crystal Diamond (SCD)Our SCD material offers extremely low strain and minimal intrinsic defects, ensuring maximum NV center stability and coherence time, essential for high-fidelity quantum applications.
Substrate Size & Thickness ControlCustom Dimensions and ThicknessWe provide SCD and PCD plates/wafers up to 125 mm in diameter. Thickness control is precise, ranging from 0.1 ”m (for thin film CL/STEM studies) up to 500 ”m.
Optimizing Plasmonic CouplingAdvanced Polishing and MetalizationSCD surfaces are polished to Ra < 1 nm, and inch-size PCD to Ra < 5 nm, enabling high-resolution lithography for plasmonic metamaterials.
Integrated Plasmonic StructuresIn-House Custom MetalizationWe offer internal deposition of critical metals (Au, Pt, Pd, Ti, W, Cu). This capability allows researchers to fabricate the optimized Ag or Au nanostructures necessary to achieve high Purcell factors (>1000) and control g(2)(τ).
Tuning Recombination DynamicsBoron-Doped Diamond (BDD) FilmsBDD allows for precise control over the Fermi level, which is critical for stabilizing the NV charge state (NV- vs. NV0) and modifying the local phonon environment to tune recombination dynamics and bunching behavior.
Global Project SupportGlobal Shipping and Engineering TeamWe offer global shipping (DDU default, DDP available) and direct consultation with our in-house PhD material scientists to assist with material selection and integration for similar Electron-Beam-Driven Quantum Emitter projects.

For custom specifications or material consultation, visit 6ccvd.com or contact our engineering team directly.

View Original Abstract

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

  1. 2017 - Advances in Imaging and Electron Physics