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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, François Treussart, Chia‐Yi Fang, Huan‐Cheng Chang, Mathieu Kociak

Published Jul 30, 2013• 19 citations
Publisher

Abstract

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.

DOI
10.1002/pssa.201300044

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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.
Abstract The numerical techniques required to prove the single‐photon emission from any type of quantum emitter (QE) after being coupled to any nanostructure are presented in this paper. The Purcell effect modifies the emission characteristics of QEs, such as color centers in nanodiamonds, for example, nitrogen‐vacancy (NV) centers, silicon vacancy (SiV) centers, and so forth, or semiconductor quantum dots. Our numerical approach is based on the unique QEs' experimental photophysics parameters and numerical analysis software, which are MATLAB and Quantum Toolbox in Python (QuTiP). Our results show a comparable g(2) (τ) behavior between our proposed numerical model and the other two experimental results for the QE before and after coupling to a plasmonic waveguide with subwavelength dimensions. Our proposed method is essential to prove the single‐photon emission of modeled single‐photon source (SPS) in an on‐chip polarization‐dependent quantum key distribution system (QKD).
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.
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.
Diamond nanocrystals containing nitrogen–vacancy (NV) color centers have been used in recent years as fluorescent probes for near-field and cellular imaging. In this work, we report that an infrared (IR) pulsed excitation beam can quench the photoluminescence of a NV color center in a diamond nanocrystal (size <50 nm) with an extinction ratio as high as ≈90%. We attribute this effect to the heating of the nanocrystal consecutive to multi-photon absorption by the diamond matrix. This quenching is reversible: the photoluminescence intensity goes back to its original value when the IR laser beam is turned off, with a typical response time of 100 ps, allowing for fast control of NV color center photoluminescence. We used this effect to achieve the sub-diffraction-limited imaging of fluorescent diamond nanocrystals on a coverglass. For that, as in the ground state depletion super-resolution technique, we combined the green excitation laser beam with the control IR depleting one after shaping its intensity profile in a doughnut form, so that the emission comes only from the sub-wavelength size central part.
Diamond nanocrystals containing highly photoluminescent color centers are attractive, nonclassical, and near-field light sources. For near-field applications, the size of the nanocrystal is crucial, since it defines the optical resolution. Nitrogen-vacancy (NV) color centers are efficiently created by proton irradiation and annealing of a nanodiamond powder. Using near-field microscopy and photon statistics measurements, we show that nanodiamonds with sizes down to 25 nm can hold a single NV color center with bright and stable photoluminescence.