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Physical Review Letters

Optimum Photoluminescence Excitation and Recharging Cycle of Single Nitrogen-Vacancy Centers in Ultrapure Diamond

Katja Beha, Anton Batalov, Neil B. Manson, Rudolf Bratschitsch, Alfred Leitenstorfer

Published Aug 30, 2012• 194 citations
Publisher

Abstract

Important features in the spectral and temporal photoluminescence excitation of single nitrogen-vacancy (NV) centers in diamond are reported at conditions relevant for quantum applications. Bidirectional switching occurs between the neutral (${\mathrm{NV}}^{0}$) and negatively charged (${\mathrm{NV}}^{\ensuremath{-}}$) states. Luminescence of ${\mathrm{NV}}^{\ensuremath{-}}$ is most efficiently triggered at a wavelength of 575 nm which ensures optimum excitation and recharging of ${\mathrm{NV}}^{0}$. The dark state of ${\mathrm{NV}}^{\ensuremath{-}}$ is identified as ${\mathrm{NV}}^{0}$. A narrow resonance is observed in the excitation spectra at 521 nm, which mediates efficient conversion to ${\mathrm{NV}}^{0}$.

DOI
10.1103/physrevlett.109.097404

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Important features in the spectral and temporal photoluminescence excitation of single nitrogen-vacancy (NV) centers in diamond are reported at conditions relevant for quantum applications. Bidirectional switching occurs between the neutral (NV0{\mathrm{NV}}^{0}NV0) and negatively charged (NV\ensuremath−{\mathrm{NV}}^{\ensuremath{-}}NV\ensuremath−) states. Luminescence of NV\ensuremath−{\mathrm{NV}}^{\ensuremath{-}}NV\ensuremath− is most efficiently triggered at a wavelength of 575 nm which ensures optimum excitation and recharging of NV0{\mathrm{NV}}^{0}NV0. The dark state of NV\ensuremath−{\mathrm{NV}}^{\ensuremath{-}}NV\ensuremath− is identified as NV0{\mathrm{NV}}^{0}NV0. A narrow resonance is observed in the excitation spectra at 521 nm, which mediates efficient conversion to NV0{\mathrm{NV}}^{0}NV0.
We report the observation of multiphoton photoluminescence excitation (PLE) below the resonant energies of nitrogen vacancy (NV) centers in diamond. The quadratic and cubic dependence of the integrated fluorescence intensity as a function of excitation power indicates a two-photon excitation pathway for the ${\mathrm{NV}}^{\ensuremath{-}}$ charge state and a three-photon process involved for the neutral NV0{\mathrm{NV}}^{0}NV0 charge state, respectively. Comparing the total multiphoton energy with its single-photon equivalent, the PLE spectra follows the absorption spectrum of single photon excitation. We also observed that the efficiency of photoluminescence for different charge states, as well as the decay time constant, was dependent on the excitation wavelength and power.
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 NV0{\mathrm{NV}}^{0}NV0 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 NV0{\mathrm{NV}}^{0}NV0 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.
Nitrogen-vacancy (NV) centers in diamond can be read out optically or electrically. To better understand the physics of their internal electronic transitions as well as ionization and recharging, we study the spin contrast observed in both readout methods as a function of the excitation wavelength for both single NV centers and ensembles. While the optical readout works best between 525 and 550 nm, the highest electrical spin contrast is achieved by resonantly exciting the NV0 zero-phonon line at 575 nm. Additional spectral features attributed to a further excited state of NV−, phonon sidebands and tunnel coupling to nitrogen donors are observed and discussed.
Nitrogen–vacancy (NV) colour centres in diamond are attractive fluorescence emitters owing to their unprecedented photostability and superior applicability to spin manipulation and sub-diffraction far-field optical microscopy. However, some applications are limited by the co-occurrence of dark state population and optical excitation. In this paper, we use fluorescence microscopy and correlation spectroscopy on single negatively charged NV centres in type IIa bulk diamond to unravel the population kinetics of a >100 s long-lived dark state. The bright–dark state interconversion rates show a quadratic dependence on the applied laser intensity, which implies that higher excited states are involved. Depopulation of the dark state becomes less effective at wavelengths above 532 nm, resulting in a complete fluorescence switch-off at wavelengths >600 nm. This switch is reversible by the addition of shorter wavelengths. This behaviour can be explained by a model consisting of three dark and three bright states of different excitation levels, with the most efficient interconversion via the respective higher excited states. This model accounts for the nonlinear dark state and photoswitching kinetics, as well as for the decrease of the NV's fluorescence lifetime with excitation intensity and the strong dependence of fluorescence emission on excitation intensity. Unfortunately, our data do not give enough insight to allow us to assign the different states to specific electronic states known from the literature. Nevertheless, our observations allowed us to improve the recording of fluorescence images of single NV centres with sub-diffraction spatial resolution but they also have important implications for studying their spin states.