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arXiv:2209.12558 · Journal of Applied Physics

High temperature spectroscopy of ensembles of nitrogen-vacancy centers in diamond

Mohammed Attrash, Oleg Shtempluck, Eyal Buks

Published Mar 1, 2023• 11 citations
arXivHTMLPDF

Abstract

We study the spectroscopy of an ensemble of negatively charged nitrogen-vacancy centers in diamond at high temperatures between room temperature and 700K under high vacuum conditions. Spin resonances are studied using optical detection of magnetic resonance (ODMR), and optical spectroscopy is employed to study radiative transitions. Upon increasing the temperature, the intensity of radiative decay in visible and infrared decreased. In addition, the ODMR resonance frequencies were decreased, and the phonon line emission shifted to higher wavelengths. Density functional theory calculation of the zero-field splitting parameter (D) revealed that thermal expansion is not enough to explain the shift in the ODMR frequencies. Fitting the measured intensity of photo-luminescence with the theoretical predictions of the Mott–Seitz model yields the value of 0.22eV for the energy barrier associated with nonradiative decay.

DOI
10.1063/5.0128069

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Journal of Applied Physics•Mar 15, 2012•1 citation
We study the spectroscopy of an ensemble of negatively charged nitrogen-vacancy centers in diamond at high temperatures between room temperature and 700K under high vacuum conditions. Spin resonances are studied using optical detection of magnetic resonance (ODMR), and optical spectroscopy is employed to study radiative transitions. Upon increasing the temperature, the intensity of radiative decay in visible and infrared decreased. In addition, the ODMR resonance frequencies were decreased, and the phonon line emission shifted to higher wavelengths. Density functional theory calculation of the zero-field splitting parameter (D) revealed that thermal expansion is not enough to explain the shift in the ODMR frequencies. Fitting the measured intensity of photo-luminescence with the theoretical predictions of the Mott–Seitz model yields the value of 0.22eV for the energy barrier associated with nonradiative decay.
The spin dynamics of the negatively charged nitrogen-vacancy (NV⁻) centers in diamond are highly sensitive to quantum electromagnetic fluctuations arising from optical excitation, chemical interactions, and thermal processes. Here we investigated the optical and spin properties of ensembles of NV⁻ centers in diamond under continuous-wave (CW) and nanosecond pulsed laser excitation. Optical detection of magnetic resonance (ODMR) is employed to monitor laser induced shifts of the zero-field splitting parameter D under ambient and high-vacuum conditions. Increasing CW laser power results in a systematic downshift of the resonance frequency due to laser-induced heating. The effect is significantly enhanced under vacuum, where the shift in D reaches up to ~17 MHz, compared to ~5 MHz in air, emphasizing the role of environmental thermal dissipation. Under nanosecond pulsed excitation, increasing the pulse repetition rate similarly leads to resonance shifts and reduced ODMR contrast, consistent with cumulative thermal effects. Visible and infrared spectroscopy confirm power dependent modifications of NV emission. Time resolved photoluminescence measurements showed that the excited-state lifetime (~6 ns) remains nearly constant across the investigated excitation range, indicating that in this regime the dominant limitation is thermal loading of the spin resonance rather than a change in intrinsic radiative decay dynamics. These results provide a comprehensive characterization of thermal effects in high power optical excitation of NV ensembles and are directly relevant for high intensity NV-based sensing and spectroscopy, particularly in vacuum environments.
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.
Magnetic resonance and fluorescence spectra of nitrogen-vacancy (NV) color centers ensemble in high purity diamond sample were measured, with temperature ranging from 5.6 K to 295 K. Both microwave and optical transition energies have similar nonlinear temperature dependent changes, which might mainly originate from the local thermal expansion. As the frequency shifts will reduce the fidelity of resonant quantum control, the present results demonstrate the necessity of taking temperature fluctuation into consideration. For temperature below 100 K, the transition energies show tendencies to be constant, which indicate higher stability and performance in applications with NV centers.
The ensemble of nitrogen-vacancy (NV) centers is widely used in quantum information transmission, high-precision magnetic field, and temperature sensing due to their advantages of long-lived state and the ability to be pumped by optical cycling. In this study, we investigate the zero-phonon line behavior of the two charge states of NV centers by measuring the photoluminescence of the NV center at 1.6 K-300 K. The results demonstrate a positional redshift, an increase in line width, and a decrease in fluorescence intensity for the ZPL of NV0 and NV- as the temperature increased. In the range of 10 K to 140 K, the peak shift with high concentrations of NV- revealed an anomaly of bandgap reforming. The peak position undergoes a blueshift and then a redshift as temperature increases. Furthermore, the transformation between NV0 and NV- with temperature changes has been obtained in diamonds with different nitrogen concentrations. This study explored the ZPL characteristics of NV centers in various temperatures, and the findings are significant for the development of high-resolution temperature sensing and high-precision magnetic field sensing in ensemble NV centers.
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.
We theoretically investigate the multiphonon effects on the optical emission spectra of the negatively charged nitrogen-vacancy (NV−) center in diamond and find that the fluorescence emission spectra described by the single frequency model agree quite well with the experimental data. From a comparison between our theory and the experimental results, we also find a reduction of the anti-Stokes shift of the emission spectra at high temperature. This is contradictory to the linear hole-phonon interaction model. We resolve this contradiction by adding the quadratic hole-phonon interaction to our model. Our theoretical analyses show that this may reduce the lattice relaxation energy. As a consequence, fewer phonons are emitted in the optical transition, therefore explaining the reduction of the anti-Stokes shift at high temperature.