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arXiv:1302.2154 · New Journal of Physics

Quenching nitrogen–vacancy center photoluminescence with an infrared pulsed laser

Ngoc Diep Lai, Orestis Faklaris, Dingwei Zheng, V. Jacques, Huan‐Cheng Chang, Jean-François Roch, François Treussart

Published Mar 22, 2013• 35 citations

Abstract

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.

DOI: 10.1088/1367-2630/15/3/033030

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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.

The effect of laser radiation with a wavelength near 1.55 µm on the photoluminescence properties of “nitrogen-vacancy” (NV) color centers in diamond has been studied experimentally. The effect of radiation of an infrared laser on the charge state of color centers redistributes the spectral intensity of photoluminescence in the ensemble of NV centers. In the case of neutral NV centers, the quenching of photoluminescence reaching about 60% has been observed. A feature of the laser excitation of NV centers by this method is the absence of competition with stimulated emission and two-photon excitation, which is observed with an increase in the power of infrared radiation at other wavelengths.

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 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.

The negatively charged nitrogen-vacancy ([Formula: see text]) centre in nanodiamonds (NDs) has been recently studied for applications in cellular imaging due to its better photo-stability and biocompatibility if compared to other fluorophores. Super-resolution imaging achieving 20-nm resolution of [Formula: see text] in NDs has been proved over the years using sub-diffraction limited imaging approaches such as single molecule stochastic localisation microscopy and stimulated emission depletion microscopy. Here we show the first demonstration of ground-state depletion (GSD) nanoscopy of these centres in NDs using three beams, a probe beam, a depletion beam and a reset beam. The depletion beam at 638 nm forces the [Formula: see text] centres to the metastable dark state everywhere but in the local minimum, while a Gaussian beam at 594 nm probes the [Formula: see text] centres and a 488-nm reset beam is used to repopulate the excited state. Super-resolution imaging of a single [Formula: see text] centre with a full width at half maximum of 36 nm is demonstrated, and two adjacent [Formula: see text] centres separated by 72 nm are resolved. GSD microscopy is here applied to [Formula: see text] in NDs with a much lower optical power compared to bulk diamond. This work demonstrates the need to control the NDs nitrogen concentration to tailor their application in super-resolution imaging methods and paves the way for studies of [Formula: see text] in NDs' nanoscale interactions.

The photophysics and charge state dynamics of the nitrogen vacancy (NV) center in diamond has been extensively investigated, but is still not fully understood. In contrast to previous work, we find that

{\mathrm{NV}}^{0}

converts to ${\mathrm{NV}}^{\ensuremath{-}}$ under excitation with low power near-infrared (1064-nm) light, resulting in increased photoluminescence from the ${\mathrm{NV}}^{\ensuremath{-}}$ state. We used a combination of spectral and time-resolved photoluminescence experiments and rate-equation modeling to conclude that

{\mathrm{NV}}^{0}

converts to ${\mathrm{NV}}^{\ensuremath{-}}$ via absorption of 1064-nm photons from the valence band of diamond. We report fast quenching and recovery of the photoluminescence from both charge states of the NV center under low power 1064-nm laser excitation, which has not been previously observed. We also find, using optically detected magnetic resonance experiments, that the charge transfer process mediated by the 1064-nm laser is spin dependent.