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Conference on Lasers and Electro-Optics

Charge switching dynamics and optimal excitation wavelength of single NV centers in ultrapure diamond

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

Published Jan 1, 2012• 0 citations
Publisher

Abstract

Photoluminescence excitation spectra of single NV centers in diamond are studied and an optimal wavelength for NV− is found. The physics of bidirectional switching between NV0 and NV− charge states of the defect is elucidated.
DOI
10.1364/qels.2012.qf1e.1

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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 (${\mathrm{NV}}^{\ensuremath{-}}$) 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.
Abstract Nitrogen-vacancy (NV) defect centers in diamond are key to applications in quantum sensing and quantum computing. They create localized electronic states in the diamond lattice with distinct population relaxation pathways following photoexcitation that ultimately enable its unique properties. The defect is known to exist in two charge states: neutral and negative, with respectively one and two known optically-active electronic transitions. Here, we report on the observation of a large number of hitherto undiscovered excited electronic states in both charge states as evidenced by distinct optical transitions in the infrared to ultraviolet part of the spectrum. These transitions are observed by monitoring the electronic relaxation of NV centers after photoexcitation using transient absorption spectroscopy, directly probing transient phenomena occurring on timescales from femtoseconds to microseconds. We also for the first time probed the electron transfer dynamics from the 3 E state of NV− to nearby single-substitutional nitrogen defects (N s ) that leads to the well-known effect of NV photoluminescence quenching.
The nitrogen–vacancy centre (NV) has drawn much attention for over a decade, yet detailed knowledge of the photophysics needs to be established. Under typical conditions, the NV can have two stable charge states, negative (NV − ) or neutral (NV 0 ), with photo-induced interconversion of these two states. Here, we present detailed studies of the ionization dynamics of single NV centres in bulk diamond at room temperature during illumination and its dependence on the excitation wavelength and power. We apply a recent method which allows us to directly measure the charge state of a single NV centre, and observe its temporal evolution. We find that the steady-state NV − population is always ⩽75% for 450–610 nm excitation wavelength. In combination with saturation measurements, we show that the optimal excitation wavelength is around 510–540 nm. Furthermore, the relative absorption cross-section of NV − is determined for 540–610 nm, revealing a double-peak structure. Finally, the energy of the NV − ground state of 2.6 eV below the conduction band is measured. These results reveal new insights into the charge state dynamics of the NV centre.
Nitrogen-vacancy (NV) centers in diamond have been exploited as reliable single-photon emitters, with applications in quantum technologies and metrology. Two charge states are known for NV centers: NV0 and NV–, with the latter being mostly studied due to its long electron spin coherence time. Therefore, control over the charge state of the NV centers is essential. However, the understanding of the dynamics between the different states still remains challenging. Here we show that electron excitation induces the conversion from NV– to NV0 through electron-induced carrier generation. We present for the first time ultrafast pump-probe cathodoluminescence spectroscopy, with electron pulses as pump, and laser pulses as probe, to prepare and read out the NV states. The experimental data is explained with a model considering carrier dynamics (0.8 ns), NV0 spontaneous emission (20 ns) and NV0NV– back transfer (500 ms). Our results provide new insights into the NV–NV0 conversion dynamics, and into the use of pump-probe cathodoluminescence as a nanoscale NV characterization tool.