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Diamond and Related Materials

Laser-induced thermal effects on ODMR in NV-ensemble diamond at ambient and vacuum

Mohammed Attrash, Tamara Amro, Ilya Simanovsky, Oleg Shtempluck, Aharon Blank, Pavel Ginzburg, Eyal Buks, Hani Barhum

Published Mar 26, 2026• 0 citations
Publisher

Abstract

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.

DOI
10.1016/j.diamond.2026.113574

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The nitrogen-vacancy (NV) centers in diamond have the advantages of stable triaxial structure, ultra-long electron spin coherence time and simple optical readout at room temperature. A nitrogen atom in the diamond crystal replaces a carbon atom and a vacancy is generated at the adjacent position, forming a point defect in the C3v space group structure. Its ground state and excited state are both spin triplet states. It is the key to achieving efficient preparation of optical initial state and extracting NV color center’s information in the researches of highly sensitive sensing magnetic detection, temperature detection, biological imaging, quantum computing, etc. However, there was no systematic study on relevant parameters of laser for high-concentration NV color center’s samples in previous experimental studies. Based on a high concentration diamond NV ensemble, we use pulsed optical detection magnetic resonance (ODMR) technology to systematically study the relationship among laser initial polarization time, information reading time and laser power, and the influence of laser incident polarization angle on the accuracy of sensing information. The effects of various laser parameters on the NV1 peak of ODMR on the [111] axis of the NVs of diamond are also investigated. The contrast of ODMR increases firstly with a sigmoid function and then decreases with an e-exponential function as the information reading time increases. The incident polarization angle of the laser is sinusoidal, with a period of 90°. According to the above experimental results, we finally choose the appropriate experimental parameters at 45.8 W/cm2 (300 μs of polarization, 700 ns, reading time, laser incident angle is 220°) for ODMR test. Compared with previous experimental parameters (polarization time was 50 us, read the time of 3000 ns, laser incident angle was 250°), the experimental results show that the contrast of ODMR increases from 2.1% to 4.6%, and the typical magnetic sensitivity is improved from 21.6 nT/Hz1/2 to 5.6 nT/Hz1/2. The optimization of the optical control of NVs in solid diamond is realized. The above results provide an effective support for the detection of high-sensitivity manipulation sensing based on high-concentration NV ensemble.

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The photophysics and charge state dynamics of the nitrogen vacancy (NV) center in diamond has been extensively investigated, but is still not fully understood. In contrast to previous work, we find that ${\mathrm{NV}}^{0}$ converts to ${\mathrm{NV}}^{\ensuremath{-}}$ under excitation with low power near-infrared (1064-nm) light, resulting in increased photoluminescence from the ${\mathrm{NV}}^{\ensuremath{-}}$ state. We used a combination of spectral and time-resolved photoluminescence experiments and rate-equation modeling to conclude that ${\mathrm{NV}}^{0}$ converts to ${\mathrm{NV}}^{\ensuremath{-}}$ via absorption of 1064-nm photons from the valence band of diamond. We report fast quenching and recovery of the photoluminescence from both charge states of the NV center under low power 1064-nm laser excitation, which has not been previously observed. We also find, using optically detected magnetic resonance experiments, that the charge transfer process mediated by the 1064-nm laser is spin dependent.

arXiv:1603.08066•Physical review. B./Physical review. B•Jul 5, 2016•56 citations
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 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.
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.
Nitrogen-vacancy (NV) centers in diamond have found broad applications owing to optical spin initialization and readout as well as long spin coherence time at room temperature.1 Recently, we have reported the construction of a pulsed optically detected magnetic resonance (ODMR) system based on double quantum (DQ) Ramsey magnetometry with lock-in (LI) detection towards DC magnetic field sensitivity sufficient for magnetoencephalography.2 The LI detection of fluorescence allowed reduction of the noise floor, removal of the signal offset, and real-time monitoring of the magnetic field. Beyond the CW-ODMR, where spectral broadening and contrast reduction are induced by high-power excitation, the DQ-Ramsey is expected to have highersensitivity, as it allows extension of spin dephasing time T2 * and increase of contrast and fluorescence rates.2 In practice, however, the magnetic sensitivity depends also on how the optical excitation is applied. In this study, we report the excitation power stabilization by reducing the phase noise and the effect of the excitation power on the fluorescence saturation behavior.
The nitrogen-vacancy (NV) centers in diamond have the advantages of stable triaxial structure, ultra-long electron spin coherence time and simple optical readout at room temperature. A nitrogen atom in the diamond crystal replaces a carbon atom and a vacancy is generated at the adjacent position, forming a point defect in the C3v space group structure. Its ground state and excited state are both spin triplet states. It is the key to achieving efficient preparation of optical initial state and extracting NV color center’s information in the researches of highly sensitive sensing magnetic detection, temperature detection, biological imaging, quantum computing, etc. However, there was no systematic study on relevant parameters of laser for high-concentration NV color center’s samples in previous experimental studies. Based on a high concentration diamond NV ensemble, we use pulsed optical detection magnetic resonance (ODMR) technology to systematically study the relationship among laser initial polarization time, information reading time and laser power, and the influence of laser incident polarization angle on the accuracy of sensing information. The effects of various laser parameters on the NV1 peak of ODMR on the [111] axis of the NVs of diamond are also investigated. The contrast of ODMR increases firstly with a sigmoid function and then decreases with an e-exponential function as the information reading time increases. The incident polarization angle of the laser is sinusoidal, with a period of 90°. According to the above experimental results, we finally choose the appropriate experimental parameters at 45.8 W/cm2 (300 μs of polarization, 700 ns, reading time, laser incident angle is 220°) for ODMR test. Compared with previous experimental parameters (polarization time was 50 us, read the time of 3000 ns, laser incident angle was 250°), the experimental results show that the contrast of ODMR increases from 2.1% to 4.6%, and the typical magnetic sensitivity is improved from 21.6 nT/Hz1/2 to 5.6 nT/Hz1/2. The optimization of the optical control of NVs in solid diamond is realized. The above results provide an effective support for the detection of high-sensitivity manipulation sensing based on high-concentration NV ensemble.
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 photophysics and charge state dynamics of the nitrogen vacancy (NV) center in diamond has been extensively investigated, but is still not fully understood. In contrast to previous work, we find that NV0{\mathrm{NV}}^{0}NV0 converts to ${\mathrm{NV}}^{\ensuremath{-}}$ under excitation with low power near-infrared (1064-nm) light, resulting in increased photoluminescence from the ${\mathrm{NV}}^{\ensuremath{-}}$ state. We used a combination of spectral and time-resolved photoluminescence experiments and rate-equation modeling to conclude that NV0{\mathrm{NV}}^{0}NV0 converts to ${\mathrm{NV}}^{\ensuremath{-}}$ via absorption of 1064-nm photons from the valence band of diamond. We report fast quenching and recovery of the photoluminescence from both charge states of the NV center under low power 1064-nm laser excitation, which has not been previously observed. We also find, using optically detected magnetic resonance experiments, that the charge transfer process mediated by the 1064-nm laser is spin dependent.