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Journal of the Chinese Chemical Society

Stimulated emission cross sections and temperature‐dependent spectral shifts of neutral nitrogen‐vacancy centers in diamonds

Teng‐I Yang, Terumitsu Azuma, Yu‐Wen Huang, Yuen Yung Hui, Cheng‐Tien Chiang, Huan‐Cheng Chang

Published Dec 19, 2022• 8 citations
Publisher

Abstract

Abstract The neutral nitrogen‐vacancy (NV0) defects in diamond are photostable color centers, suitable for a wide range of applications in science and engineering. However, the photophysical properties of the centers have not yet been fully characterized. This work measured the stimulated emission cross sections of NV0 in a single‐crystal diamond by two‐photon excitation of its matrix at 344 nm. From the measured photoluminescence spectrum and the fluorescence lifetime of 20 ± 1 ns, we determined a peak stimulated emission cross section of 1.43 ± 0.07 × 10−17 cm2 at 650 nm for the NV0 centers. In addition, we have also examined the thermal shifts of the zero‐phonon line of NV0 centers in nanoscale diamonds (~100 nm in diameter) over the temperature range of 30–120°C. A temperature measurement sensitivity of 0.2 K·Hz−1/2 was achieved, which is about two‐fold better than that of NV−, despite that the fluorescence intensity of NV0 is about six‐fold lower than that of NV− in the same nanoparticles. The result is attributed to the smaller electron–phonon coupling strength of the neutral center, compared with its negatively charged counterpart.

DOI
10.1002/jccs.202200501

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Abstract The neutral nitrogen‐vacancy (NV0) defects in diamond are photostable color centers, suitable for a wide range of applications in science and engineering. However, the photophysical properties of the centers have not yet been fully characterized. This work measured the stimulated emission cross sections of NV0 in a single‐crystal diamond by two‐photon excitation of its matrix at 344 nm. From the measured photoluminescence spectrum and the fluorescence lifetime of 20 ± 1 ns, we determined a peak stimulated emission cross section of 1.43 ± 0.07 × 10−17 cm2 at 650 nm for the NV0 centers. In addition, we have also examined the thermal shifts of the zero‐phonon line of NV0 centers in nanoscale diamonds (~100 nm in diameter) over the temperature range of 30–120°C. A temperature measurement sensitivity of 0.2 K·Hz−1/2 was achieved, which is about two‐fold better than that of NV−, despite that the fluorescence intensity of NV0 is about six‐fold lower than that of NV− in the same nanoparticles. The result is attributed to the smaller electron–phonon coupling strength of the neutral center, compared with its negatively charged counterpart.
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.
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.
Stimulated emission is the process fundamental to laser operation, thereby producing coherent photon output. Despite negatively charged nitrogen-vacancy (NV−) centres being discussed as a potential laser medium since the 1980s, there have been no definitive observations of stimulated emission from ensembles of NV− to date. Here we show both theoretical and experimental evidence for stimulated emission from NV− using light in the phonon sidebands around 700 nm. Furthermore, we show the transition from stimulated emission to photoionization as the stimulating laser wavelength is reduced from 700 to 620 nm. While lasing at the zero-phonon line is suppressed by ionization, our results open the possibility of diamond lasers based on NV− centres, tuneable over the phonon sideband. This broadens the applications of NV− magnetometers from single centre nanoscale sensors to a new generation of ultra-precise ensemble laser sensors, which exploit the contrast and signal amplification of a lasing system. Here Jeskeet al. show both theoretical and experimental evidence for stimulated emission from negatively charged nitrogen vacancy centres using light in the phonon sidebands around 700 nm, demonstrating its suitability as a laser medium.
In this paper, prospects of using diamond with NV− centers as a gain medium have been studied. Spectroscopic characterization of NV− centers in diamond as well as absorption saturation and pump-probe experiments have been carried out. Absorption and emission cross-sections were estimated to be 2.8 × 10-17 cm2 and 4.3 × 10-17 cm2 at the maximum of absorption and emission bands, respectively. It was observed from emission spectra under pulse excitation that some NV− are photoionized to NV0 centers with ZPL at 575 nm. Room temperature luminescence lifetime of NV− centers was measured to be 12ns, which is close to the previously reported lifetime in bulk diamond (~13ns). Saturated transmission was only about 11% of calculated values even at energy fluence much higher than the saturation flux. Two excited state absorptions (ESAs) with different relaxation times (“fast-decay” and “slow-decay with relaxation times of ~500 ns and several tens of microseconds, respectively) were revealed in transmission decay kinetics at 632 nm. Kinetics of transmission at 670 nm was dominated by “slow-decay” ESA process. Kinetics of dk/k0 in shorter wavelength were strongly dominated by “fast-decay” ESA process. These results definitively indicate that stimulated emission of NV− centers is suppressed by photoionization and ESAs and the possibility of diamond lasers based on NV− centers is low.
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.
A study of the photophysical properties of nitrogen-vacancy (NV) color centers in diamond nanocrystals of size 50 nm or below is carried out by means of second-order time-intensity photon correlation and cross-correlation measurements as a function of the excitation power for both pure charge states, neutral and negatively charged, as well as for the photochromic state, where the center switches between both states at any power. A dedicated three-level model implying a shelving level is developed to extract the relevant photophysical parameters coupling all three levels. Our analysis confirms the very existence of the shelving level for the neutral NV center. It is found that it plays a negligible role on the photophysics of this center, whereas it is responsible for an increasing photon bunching behavior of the negative NV center with increasing power. From the photophysical parameters, we infer a quantum efficiency for both centers, showing that it remains close to unity for the neutral center over the entire power range, whereas it drops with increasing power from near unity to approximately 0.5 for the negative center. The photophysics of the photochromic center reveals a rich phenomenology that is to a large extent dominated by that of the negative state, in agreement with the excess charge release of the negative center being much slower than the photon emission process.