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arXiv:2307.11830

Wavelength Dependence of the Electrical and Optical Readout of NV Centers in Diamond

Lina M. Todenhagen, Martin S. Brandt

Published Jul 21, 2023• 0 citations
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Abstract

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$^-$.

DOI
10.48550/arxiv.2307.11830

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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−^-−.
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 optically detected magnetic resonance (ODMR) in diamond ${\mathrm{NV}}^{\ensuremath{-}}$ centers at cryogenic temperatures. We find that when we use resonant optical excitation at zero phonon line wavelength, turning on microwave radiation leads to an increase in fluorescence. This is different from the conventional case of nonresonant optical pumping where microwave radiation instead leads to a decrease in fluorescence. In addition, we observe a significant increase in contrast compared to the nonresonant ODMR. To explain this effect, we propose a theoretical model based on the interaction of the resonant optical radiation with different groups from the inhomogeneously broadened ensemble of ${\mathrm{NV}}^{\ensuremath{-}}$ centers. We find that the effect is temperature dependant and can only be observed at temperatures below 35 K.
Optical illumination on negatively charged nitrogen-vacancy $(\mathrm{N}{\mathrm{V}}^{\ensuremath{-}})$ centers inevitably causes stochastic charge-state transitions between the $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ and the neutral charge state of the NV center. It limits the steady-state population of $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ to 5% at minimum (\ensuremath{\sim}610 nm) and 80% (\ensuremath{\sim}532 nm) at maximum in intrinsic diamond depending on the wavelength. Here, we show Fermi-level control by phosphorus doping generates 99.4 \ifmmode\pm\else\textpm\fi{} 0.1% $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ under 1-\ensuremath{\mu}W and 593-nm excitation which is close to maximum absorption of $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$. The pure $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ shows a fivefold increase in luminescence and a fourfold enhancement of an optically detected magnetic resonance under 593-nm excitation compared with those in intrinsic diamond.
As promising quantum sensors, nitrogen-vacancy (N-VVV) centers in diamond have been widely used in frontier studies in condensed-matter physics, material science, and life sciences. In practical applications, weak laser excitation is favorable as it reduces the side effects of laser irradiation, such as phototoxicity and heating. Here we report a combined theoretical and experimental study of (near) zero-field optically detected magnetic resonance (ODMR) of N-VVV-center ensembles under weak 532-nm laser excitation. In this region, both the width and splitting of the ODMR spectra decrease with increasing laser power. This power dependence is reproduced with a model that accounts for the laser-induced charge neutralization of $\mathrm{N}\text{\ensuremath{-}}{V}^{\ensuremath{-}}$--N+{\mathrm{N}}^{+}N+ pairs, which alters the local electric field environment. These results are useful for the understanding and development of N-VVV-based quantum sensing in light-sensitive applications.
Magnetometry with nitrogen-vacancy (NV) centers in diamond has so far been measured via emission of light from NV centers or via absorption at the singlet transition at 1042 nm. Here, we demonstrate a phenomenon of broadband optical absorption by the NV centers starting in the emission wavelength and reaching up to 1000 nm. The measurements are enabled by a high-finesse cavity, which is used for room-temperature continuous wave pump-probe experiments. The red to infrared probe beam shows the typical optically detected magnetic resonance (ODMR) signal of the NV spin with contrasts up to 42 %. This broadband optical absorption has not yet been reported in terms of NV magnetometry. We argue that the lower level of the absorbing transition could be the energetically lower NV singlet state, based on the increased optical absorption for a resonant microwave field and the spectral behavior. Investigations of the photon-shot-noise-limited sensitivity show improvements with increasing probe wavelength, reaching an optimum of 7.5pT/Hz. The results show significantly improved ODMR contrast compared to emission-based magnetometry. This opens a new detection wavelength regime with coherent laser signal detection for high-sensitivity NV magnetometry.
The core issue for the implementation of NV center qubit technology is a sensitive readout of the NV spin state. We present here a detailed theoretical and experimental study of NV center photoionization processes, used as a basis for the design of a dual-beam photoelectric method for the detection of NV magnetic resonances (PDMR). This scheme, based on NV one-photon ionization, is significantly more efficient than the previously reported single-beam excitation scheme. We demonstrate this technique on small ensembles of $\ensuremath{\sim}10$ shallow NVs implanted in electronic grade diamond (a relevant material for quantum technology), on which we achieve a cw magnetic resonance contrast of 9%---three times enhanced compared to previous work. The dual-beam PDMR scheme allows independent control of the photoionization rate and spin magnetic resonance contrast. Under a similar excitation, we obtain a significantly higher photocurrent, and thus an improved signal-to-noise ratio, compared to single-beam PDMR. Finally, this scheme is predicted to enhance magnetic resonance contrast in the case of samples with a high proportion of substitutional nitrogen defects, and could therefore enable the photoelectric readout of single NV spins.