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Chemical Physics Letters

Quantitative luminescence microscopy on Nitrogen-Vacancy Centres in diamond: Saturation effects under pulsed excitation

Robert Chapman, Taras Plakhotnik

Published Apr 1, 2011• 48 citations
Publisher
DOI
10.1016/j.cplett.2011.03.057

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The photoluminescence of the negatively charged nitrogen-vacancy (${\mathrm{NV}}^{\ensuremath{-}}$) center displays anomalous saturation behavior at high excitation pulse energies. Where the luminescence is expected to approach a maximum value asymptotically, we have found that it instead drops by as much as a factor of two. In this report, we present evidence that these effects are caused by optical spin depolarization of the ${\mathrm{NV}}^{\ensuremath{-}}$ center. We show that the presence of an external magnetic field results in a marked decrease in the anomalous character of the ${\mathrm{NV}}^{\ensuremath{-}}$ centers' luminescence and demonstrate that low-energy pulses applied after a strong depolarizing pulse can repolarize the spin of the center. We also offer a model and derive important parameters describing dynamics in the NV center and its interaction with light, which quantitatively explain all the observations.
Optical experiments, involving photoluminescence (PL), the PL excitation and quenching spectra, as well as transmission and its quenching, were used to analyse the photochromic behaviour of some vacancy-related complexes in diamond. The 2.156 eV, 1.945 eV and 1.68 eV optical centres in CVD diamond are attributed to the neutral nitrogen-vacancy, negative nitrogen-vacancy and neutral silicon-vacancy ([Si-V](0)) centres, respectively. Oscillatory behaviour in the excitation spectrum of the 1.68 eV luminescence is observed and from the threshold of the oscillations a position of Ec - 2.05 eV is suggested for the ground state of the [Si-V](0) centre.
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.