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Functional Diamond

Observation of optical gain from NV − center in diamond by femtosecond transient absorption

Chao Fang, Wenhao Wang, Qing Lou, Liangchao Chen, Yongsheng Hu, Chongxin Shan

Published Jan 10, 2025• 1 citation
Publisher

Abstract

Single crystal diamonds with strong NV− luminescence were prepared by high-pressure high-temperature method and followed by electron irradiation and annealing process. The stimulated emission and gain characteristics of NV− diamond in femtosecond time scale are also studied using the transient absorption technique. Stimulated emission was observed at 660–800 nm, with an optical gain displayed in the range of 680–725 nm. Further test revealed that the optical gain lifetime is 3.5 ns and the gain coefficient is 0.16 cm−1, demonstrating the potential realization of color center lasers.

DOI
10.1080/26941112.2024.2449373

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Single crystal diamonds with strong NV− luminescence were prepared by high-pressure high-temperature method and followed by electron irradiation and annealing process. The stimulated emission and gain characteristics of NV− diamond in femtosecond time scale are also studied using the transient absorption technique. Stimulated emission was observed at 660–800 nm, with an optical gain displayed in the range of 680–725 nm. Further test revealed that the optical gain lifetime is 3.5 ns and the gain coefficient is 0.16 cm−1, demonstrating the potential realization of color center lasers.
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.
In this work, we focus on the interaction of SiV color centers in diamond with femtose- cond light pulses. In the theoretical part, a script is developed to simulate the experimen- tal varying stripe length method and the effects of saturated optical gain are investigated. In the experimental part, photoluminescence and transient differential absorption under non-resonant excitation are studied. The result of the luminescence measurements are estimates of the effective cross-sections of single-photon absorption for the wavelengths 620 nm, 515 nm and 340 nm, as well as the effective cross-section of three-photon absorp- tion for 2000 nm. The result of the differential absorption measurements is the relaxation constant of the excited level of the SiV center and the upper estimate of the time duration of the initial dynamics. 1
In this work, we focus on the interaction of SiV color centers in diamond with femtose- cond light pulses. In the theoretical part, a script is developed to simulate the experimen- tal varying stripe length method and the effects of saturated optical gain are investigated. In the experimental part, photoluminescence and transient differential absorption under non-resonant excitation are studied. The result of the luminescence measurements are estimates of the effective cross-sections of single-photon absorption for the wavelengths 620 nm, 515 nm and 340 nm, as well as the effective cross-section of three-photon absorp- tion for 2000 nm. The result of the differential absorption measurements is the relaxation constant of the excited level of the SiV center and the upper estimate of the time duration of the initial dynamics. 1
In this paper, we analyse the prospects for using nitrogen-vacancy centre (NV) containing diamond as a laser gain material by measuring its key laser related parameters. Synthetic chemical vapour deposition grown diamond samples with an NV concentration of ~1 ppm have been selected because of their relatively high NV concentration and low background absorption in comparison to other samples available to us. For the samples measured, the luminescence lifetimes of the NV- and NV0 centres were measured to be 8±1 ns and 20±1 ns respectively. The respective peak stimulated emission cross-sections were (3.6±0.1)×10-17 cm2 and (1.7±0.1)×10-17 cm2. These measurements were combined with absorption measurements to calculate the gain spectra for NV- and NV0 for differing inversion levels. Such calculations indicate that gains approaching those required for laser operation may be possible with one of the samples tested and for the NV- centre.
Diamond color centers such as the nitrogen-vacancy (NV) center have been extensively studied as a popular platform that enables quantum sensing and computing applications. For highly sensitive sensing NV ensembles have significantly stronger signals than individual NV centers and can create strong light fields, which are also essentially required by novel concepts that need a large sensing volume, such as cavity coupling and readout, laser threshold magnetometry and multi-pass geometries. On top of strong signals, low optical material losses are the other key consideration for these techniques, by means of low optical absorption of signal light and low birefringence of the diamond crystal. In this work, we study systematically the behavior of absorption in the NV emission range around 700nm and birefringence with increasing nitrogen- and NV-doping, as well as their behavior during NV creation via diamond growth, electron beam irradiation and annealing treatments. Absorption correlates with increased nitrogen-doping yet single substitutional nitrogen atoms (Ns0 or P1 centers) do not seem to be the direct absorber. The high nitrogen doping level in the growth leads to high absorption in the whole UV-Vis range, which is the main contributors to the high absorption at 700 nm. When treating the diamond for an enhanced NV concentration, ‘over irradiating’ the diamond with too high fluence is harmful in the sense of creating neutral vacancies that increase absorption at the wavelength range of interest. Opposite to the absorption, birefringence reduces with increasing nitrogen doping and shows better homogeneity. After-growth treatments show a minor and if any a positive (i.e. reducing) influence on diamond birefringence. Multiple crystal defect concentrations and their changes are identified via absorption spectroscopy during the material processing steps and thus we identify potential causes of absorption and birefringence. From this we suggest strategies to fabricate CVD diamonds with high NV density yet low absorption and low birefringence
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.