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SPIE Solid State Lasers: Technology and Devices

Laser spectroscopy of highly doped NV- centers in diamond

Shova D. Subedi, Jeremy M. Peppers, Sergey Mirov, Vladimir V. Federov, Dmitry V. Martyshkin, Linbo Shao, Marko Lončar

Published Feb 20, 2018• 8 citations
Publisher

Abstract

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.

DOI
10.1117/12.2290705

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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.
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.
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, 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.
We report on the spectroscopic characterization, absorption saturation, and excited-state dynamics of GR1 centers in synthetic diamonds. The non-linear optical measurements reveal an efficient bleaching of the GR1 center’s ground level under ns-pulsed 633 nm excitation. The maxima of absorption and emission cross sections were estimated to be 4.5 × 10−17 cm2 and 9 × 10−17 cm2 at 630 nm and 780 nm, respectively. The radiative lifetime of the excited level was estimated to be 8.5 ns. The 658 nm probe kinetics uncovered relaxation of 1T2 excited level going predominantly to a metastable state with a lifetime of 220 μs. An induced absorption detected with the use of a highly concentrated diamond sample could be due to up-conversion and photoionization processes in additional impurity-vacancy center with absorption at the short-wavelength tail of GR1. The results presented here indicate that synthetic diamonds with GR1 centers could serve as near infrared gain media or passive Q-switchers for laser cavities over the 633–750 nm spectral range. Optimization of the center concentration and the crystal parameters are required to minimize the induced absorption at the lasing wavelengths.