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AIP conference proceedings

Recharging dynamics of single nitrogen-vacancy centers in ultrapure diamond

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

Published Jan 1, 2013• 0 citations
Publisher

Abstract

Photoluminescence excitation spectra of individual nitrogen-vacancy (NV) centers in diamond are investigated. Recharging dynamics between the neutral (NV0) and negatively charged (NV−) states are elucidated and the optimal excitation wavelength for NV− is found. A sharp resonance at an excitation wavelength of 521 nm facilitates an efficient conversion to NV0.

DOI
10.1063/1.4848517

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Photoluminescence excitation spectra of individual nitrogen-vacancy (NV) centers in diamond are investigated. Recharging dynamics between the neutral (NV0) and negatively charged (NV−) states are elucidated and the optimal excitation wavelength for NV− is found. A sharp resonance at an excitation wavelength of 521 nm facilitates an efficient conversion to NV0.
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 (${\mathrm{NV}}^{\ensuremath{-}}$) states. Luminescence of ${\mathrm{NV}}^{\ensuremath{-}}$ is most efficiently triggered at a wavelength of 575 nm which ensures optimum excitation and recharging of NV0{\mathrm{NV}}^{0}NV0. The dark state of ${\mathrm{NV}}^{\ensuremath{-}}$ 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.
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.
We report on the spectroscopic and laser characterization of negatively charged nitrogen-vacancy (NV−) centers in diamond. Spectroscopic properties such as absorption and emission spectra as well as kinetics were studied, and parameters such as cross-sections and lifetimes were estimated. A vibronic band of NV0 with zero phonon line (ZPL) at 575 nm was detected under 532 nm pulsed excitation due to the photoionization of NV−. Transmission of 532 nm pump pulses saturate around ∼10%, which is much smaller than the theoretical level. Δk/k0 kinetics revealed slow recovery of NV− centers after photoionization under 532 nm pumping, which involved different relaxation channels depending on the probe beam wavelengths. Localization of the electrons in the metastable state of NV0 centers resulted in higher saturated transmission of 632 nm pump.
Nitrogen vacancy (NV) centers in diamond are at the heart of many emerging quantum technologies, all of which require control over the NV charge state. Hence, methods for quantification of the relative photoluminescence intensities of the NV0 and NV− charge states, i.e., a charge state ratio, are vital. Several approaches to quantify NV charge state ratios have been reported but are either limited to bulk-like NV diamond samples or yield qualitative results. We propose an NV charge state quantification protocol based on the determination of sample- and experimental setup-specific NV0 and NV− reference spectra. The approach employs blue (400–470 nm) and green (480–570 nm) excitation to infer pure NV0 and NV− spectra, which are then used to quantify NV charge state ratios in subsequent experiments via least squares fitting. We test our dual excitation protocol (DEP) for a bulk diamond NV sample and 20 and 100 nm nanodiamond particles and compare results with those obtained via other commonly used techniques such as zero-phonon line fitting and non-negative matrix factorization. We find that DEP can be employed across different samples and experimental setups and yields consistent and quantitative results for NV charge state ratios that are in agreement with our understanding of NV photophysics. By providing robust NV charge state quantification across sample types and measurement platforms, DEP will support the development of NV-based quantum technologies.
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.