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arXiv:2411.10638 · Physical Review Letters

Nonlinear optical charge-state switching and pumping to dark state of a diamond nitrogen-vacancy center

Prasoon Kumar Shandilya, Vinaya K. Kavatamane, Sigurd Flågan, David P. Lake, Денис Дмитриевич Сукачев, Paul E. Barclay

Published Oct 26, 2026• 1 citation
arXivHTMLPDF

Abstract

The photodynamics of diamond nitrogen-vacancy (NV) centers limits their performance in many quantum technologies. Quenching of photoluminescence, which degrades NV readout, is commonly ascribed to a dark state that is not fully understood. Using a nanoscale cavity to generate intense infrared fields that quench NV emission nonlinearly with field intensity, we show that the dark state is accessed by two-photon pumping into the $^4\!A_2$ quartet state of the neutrally charged NV (NV$^0$). We constrain this state's energy relative to the NV$^0$ ground-state ($^2\!E$) to ${<}0.58$\,eV and the recombination energy threshold to the NV$^-$ ground state ($^3\!A_2$) to $\leq2.33\,\text{eV}$. Furthermore, we estimate the intrinsic lifetime of $^4\!A_2$ state to be $1.78-6.06\,μ\text{s}$ and show that accessing this state allows sensing of local infrared fields. This new understanding will allow predictions of the limits of NV technologies reliant upon intense fields, including levitated systems, spin--optomechanical devices, and absorption--based magnetometers.

DOI
10.1103/fjhl-yd66

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The photodynamics of diamond nitrogen-vacancy (NV) centers limits their performance in many quantum technologies. Quenching of photoluminescence, which degrades NV readout, is commonly ascribed to a dark state that is not fully understood. Using a nanoscale cavity to generate intense infrared fields that quench NV emission nonlinearly with field intensity, we show that the dark state is accessed by two-photon pumping into the 4 ⁣A2^4\!A_24A2​ quartet state of the neutrally charged NV (NV0^00). We constrain this state's energy relative to the NV0^00 ground-state (2 ⁣E^2\!E2E) to <0.58{<}0.58<0.58,eV and the recombination energy threshold to the NV−^-− ground state (3 ⁣A2^3\!A_23A2​) to ≤2.33 eV\leq2.33\,\text{eV}≤2.33eV. Furthermore, we estimate the intrinsic lifetime of 4 ⁣A2^4\!A_24A2​ state to be 1.78−6.06 μs1.78-6.06\,μ\text{s}1.78−6.06μs and show that accessing this state allows sensing of local infrared fields. This new understanding will allow predictions of the limits of NV technologies reliant upon intense fields, including levitated systems, spin--optomechanical devices, and absorption--based magnetometers.
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.
Negatively charged nitrogen-vacancy (NV${}^{\ensuremath{-}}$) color centers in diamond have generated much interest for use in quantum technology. Despite the progress made in developing their applications, many questions about the basic properties of NV${}^{\ensuremath{-}}$ centers remain unresolved. Understanding these properties can validate theoretical models of NV${}^{\ensuremath{-}}$, improve their use in applications, and support their development into competitive quantum devices. In particular, knowledge of the phonon modes of the 1A1{}^{1}{A}_{1}1A1​ electronic state is key for understanding the optical pumping process. Using pump-probe spectroscopy, we measured the phonon sideband of the ${}^{1}E\ensuremath{\rightarrow}{}^{1}{A}_{1}$ electronic transition in the NV${}^{\ensuremath{-}}$ center. From this we calculated the ${}^{1}E\ensuremath{\rightarrow}{}^{1}{A}_{1}$ one-phonon absorption spectrum and found it to differ from that of the ${}^{3}E\ensuremath{\rightarrow}{}^{3}{A}_{2}$ transition, a result which is not anticipated by previous group-theoretical models of the NV${}^{\ensuremath{-}}$ electronic states. We identified a high-energy 169-meV localized phonon mode of the 1A1{}^{1}{A}_{1}1A1​ level.
Nitrogen vacancy (NV) centers in diamond have been identified over the past few years as promising systems for a variety of applications, ranging from quantum information science to magnetic sensing. This relies on the unique optical and spin properties of the negatively charged NV. Many of these applications require shallow NV centers, i.e., NVs that are close (a few nm) to the diamond surface. In recent years there has been increasing interest in understanding the spin and charge dynamics of NV centers under various illumination conditions, specifically under infrared (IR) excitation, which has been demonstrated to have significant impact on the NV centers' emission and charge state. Nevertheless, a full understanding of all experimental data is still lacking, with further complications arising from potential differences between the photodynamics of bulk and shallow NVs. Here we suggest a generalized quantitative model for NV center spin- and charge-state dynamics under both green and IR excitation. We experimentally extract the relevant transition rates, providing a comprehensive model which reconciles all existing experimental results in the literature, except for highly nonlinear regimes. Moreover, we identify key differences between the photodynamics of bulk and shallow NVs, and use them to significantly enhance the initialization fidelity of shallow NVs to the useful negatively charged state.
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 positively charged nitrogen vacancy (NV+) center in diamond has been traditionally treated as a dark state due to the experimental lack of an optical signature. Recent computational studies have shown that it is possible for the NV+ defect to have an excited state transition equivalent to that of the negatively charged (NV−) center, but no photoluminescence (PL) predictions have been reported so far. We report the first ab initio calculation showing that the NV+ center presents quantum emission, with zero phonon line at 765 nm and a non-zero transition dipole moment, approximately one quarter of the transition dipole moment of NV−. We calculate the energy levels of the multielectron states under the time-dependent density functional theory (singlet and triplet E states), and using our recently developed frequency cutoff method, we predict the full PL spectrum. Our results suggest that this state cannot be considered intrinsically “dark” and charge specific quenching mechanisms should be investigated as the cause of the lack of optical activity in experimental characterizations.
Diamond nanocrystals containing nitrogen–vacancy (NV) color centers have been used in recent years as fluorescent probes for near-field and cellular imaging. In this work, we report that an infrared (IR) pulsed excitation beam can quench the photoluminescence of a NV color center in a diamond nanocrystal (size <50 nm) with an extinction ratio as high as ≈90%. We attribute this effect to the heating of the nanocrystal consecutive to multi-photon absorption by the diamond matrix. This quenching is reversible: the photoluminescence intensity goes back to its original value when the IR laser beam is turned off, with a typical response time of 100 ps, allowing for fast control of NV color center photoluminescence. We used this effect to achieve the sub-diffraction-limited imaging of fluorescent diamond nanocrystals on a coverglass. For that, as in the ground state depletion super-resolution technique, we combined the green excitation laser beam with the control IR depleting one after shaping its intensity profile in a doughnut form, so that the emission comes only from the sub-wavelength size central part.