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arXiv:1107.0502

Diamond particles as nanoantennas for nitrogen-vacancy color centers

Jean‐Jacques Greffet, Jean‐Paul Hugonin, Mondher Besbes, Ngoc Diep Lai, François Treussart, Jean-François Roch

Published Jul 3, 2011• 19 citations
arXivHTMLPDF

Abstract

The photoluminescence of nitrogen-vacancy (NV) centers in diamond nanoparticles exhibits specific properties as compared to NV centers in bulk diamond. For instance large fluctuations of lifetime and brightness from particle to particle have been reported. It has also been observed that for nanocrystals much smaller than the mean luminescence wavelength, the particle size sets a lower threshold for resolution in Stimulated Emission Depletion (STED) microscopy. We show that all these features can be quantitatively understood by realizing that the absorption-emission of light by the NV center is mediated by the diamond nanoparticle which behaves as a dielectric nanoantenna.

DOI
10.48550/arxiv.1107.0502

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The photoluminescence of nitrogen-vacancy (NV) centers in diamond nanoparticles exhibits specific properties as compared to NV centers in bulk diamond. For instance large fluctuations of lifetime and brightness from particle to particle have been reported. It has also been observed that for nanocrystals much smaller than the mean luminescence wavelength, the particle size sets a lower threshold for resolution in Stimulated Emission Depletion (STED) microscopy. We show that all these features can be quantitatively understood by realizing that the absorption-emission of light by the NV center is mediated by the diamond nanoparticle which behaves as a dielectric nanoantenna.
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.
Fluorescent nitrogen vacancies (NV) in diamond have drawn much interest because of their potential for computation and quantum cryptography, as well as for nanoscale magnetic imaging and biolabeling due to their special spin and fluorescence properties. However, their optical detection and control is compromised by the diffraction resolution barrier of far-field optics. We showed that stimulated emission depletion (STED) microscopy is capable of imaging NV centres with nanoscale resolution and Ångström precision using focused visible light [1].
The resonant high-index nanostructures open opportunities for control many optical effects via optically-induced electric and magnetic Mie resonances, mostly localized inside the structures. Especial interest such nanostructures represent for quantum emitters placed inside, that makes possible enhancement of quantum source emission through resonant coupling to localized modes. We have proposed the concept of active dielectric nanoantennas based on nanodiamonds with embedded NV-centers. The study of theoretically dependence of optical properties of this system on the spectral position of the resonant modes has demonstrated that that at some sizes of the diamond spherical particles and certain position of the dipole in the sphere the Purcell factor can achieve the value of 30. We have demonstrated experimentally that the photoluminescence properties of the NV-centers can be controlled via scattering resonances and observed a decrease of the NV-centers lifetime in the studied diamond particles, as compared to nonresonant nanodiamonds. These results are in a good agreement with our theoretical calculations for the average Purcell factor for multiple NV-centers within a nanoparticle. The simplicity of the proposed concept compared to existing photonic cavity systems and applicability for a wide range of color centers in diamond make active diamond nanoantenna an effective tool for creating controllable emitting elements in the visible range for future nanophotonic devices.
We investigate diamond nitrogen-vacancy (NV) centers as alternative labels in stimulated emission depletion (STED) microscopy. To this end, artificial diamond is used as a substrate and Raman spectroscopy in photoluminescence (PL) mode is performed for clearly identifying the emission wavelengths of the NV centers. With the aid of a STED microscopy system, we imaged a random feature on substrate surface with the NV-centers in STED and confocal mode. Our first measurements indicate that the combination of NV centers and STED is very promising for resolving the structures and can be further extended to nanoscale structures applied on the diamond substrates.
Charged nitrogen-vacancy (NV) color centers in diamond are excellent luminescence sources for far-field fluorescence nanoscopy by stimulated emission depletion (STED). Here we show that these photostable color centers can be visualized by STED using simple continuous-wave or high repetition pulsed lasers (76 MHz) at wavelengths >700 nm for STED. Furthermore, we show that NV centers can be imaged in three dimensions (3D) inside the diamond crystal and present single-photon signatures of single color centers recorded in high density samples, demonstrating a new recording scheme for STED and related far-field nanoscopy approaches. Finally, we exemplify the potential of using nanodiamonds containing NV centers as luminescence tags in STED microscopy. Our results offer new experimental avenues in nanooptics, nanotechnology, and the life sciences.
The development of reliable devices to generate single photons is crucial for applications in quantum cryptography, as well as for fundamental quantum optics experiments. Due to their extremely high photostability at room temperature, optically active defects in solids, the so called color centers, are among the most promising candidates. Single NV (nitrogen-vacancy) centers in diamond have been demonstrated to be able to generate single photons and have already shown advantages compared to attenuated laser pulses in a quantum cryptography experiment. The nitrogen-vacancy center (NV center) in diamond consists of a substitutional nitrogen atom and an adjacent vacancy. This complex exhibits an optical transition with a fluorescence lifetime of 11.6 ns. The room temperature spectrum of the NV center consists of the zero-phonon line at 637 nm and broad phononic sidebands with a FWHM of more than 100 nm. Due to the existence of a shelving level the efficiency of the NV center as a single photon source is limited. Additionally, the high diffraction index of bulk diamond restricts the efficiency to collect the fluorescence light.