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Applied Physics Letters

Optical and electrical readout of diamond NV centers in dependence of the excitation wavelength

Lina M. Todenhagen, Martin S. Brandt

Published May 12, 2025• 4 citations
Publisher

Abstract

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.

DOI
10.1063/5.0264362

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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 study the contrast for electrical and optical readout of NV centers in diamond in dependence of the optical excitation wavelength using different excitation schemes. While the optically detected magnetic resonance (ODMR) works efficiently between 480 and 580 nm, electrically detected magnetic resonance (EDMR) shows a strong dependence on the excitation dynamics. The highest, electrically detected contrast of -23% is achieved by resonantly exciting the zero-phonon line of the neutral charge state of NV at 575 nm. EDMR is also enhanced at 521 nm, possibly due to a further excited state of NV−^-−.
The nitrogen-vacancy (NV) center in diamond enables optical initialization and readout of its electronic spin, forming the basis of a wide range of quantum sensing and metrology applications. A central challenge in such measurements is the coexistence of two charge states, NV- and NV0: While detection protocols rely on the spin-dependent properties of NV-, fluorescence from NV0 does not carry useful contrast and is typically removed as background, reducing the available signal. Here, we show that the origin of NV0 emission depends strongly on the excitation wavelength in nitrogen-containing diamond. Using ensembles of NV centers with varying nitrogen concentrations, we compare excitation at the NV0 zero-phonon line (ZPL) at 575 nm with the commonly used 532 nm. We find that excitation at 575 nm generates NV0 predominantly through spin-selective tunneling from the excited state of NV- to nearby nitrogen donors, such that the NV0 emission follows the spin polarization of NV-. As a result, the NV0 fluorescence contributes to the measurable spin contrast, allowing the full fluorescence signal to be used for detection. This result opens opportunities for improved sensitivity in NV-based sensing applications.
Nitrogen-vacancy (NV) centers in single-crystal CVD diamond are promising candidates for quantum sensing due to their remarkable optical and spin properties [1]. These defects exhibit stable photoluminescence (PL), long spin coherence times, and high sensitivity to external fields [2]. In this study, we present a room-temperature PL characterization of NV centers excited with a 532 nm laser. The setup was optimized for high signal-to-noise ratio and spectral resolution. Key parameters analyzed include emission intensity, zero-phonon line (ZPL) at ~637 nm, phonon sidebands, and the charge state distribution between NV⁰ and NV⁻. The NV⁻ state, crucial for spin-based sensing, is evaluated to understand its stability under different nitrogen doping conditions [3]. The relative intensities of NV⁰ and NV⁻ provide insights into nitrogen incorporation and vacancy formation. These results contribute to optimizing synthesis conditions for enhanced NV⁻ concentration, supporting the advancement of diamond-based quantum sensing technologies.
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.
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.