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SPIE Solid State Lasers: Technology and Devices

Study of relaxation dynamics of excited state of GR1 centers in diamond

Shova D. Subedi, Vladimir Fedorov, Sergey Mirov, Matthew Markham

Published Mar 4, 2021• 0 citations
Publisher

Abstract

We study the decay kinetics of excited state of GR1 center in diamond using 633 nm pump pulse and 658 nm CW probe beam. The absorption saturation followed by a strong absorption of the probe below steady-state transmission level was observed. The recovery of the centers to the original level occurs slowly with ~500 ns time scale and reveals multi-exponential rates with no long-term bleaching or residual absorption. The branching ratio for relaxation process to the ground state and to the metastable state was estimated to be ~ 0.50.

DOI
10.1117/12.2583168

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We study the decay kinetics of excited state of GR1 center in diamond using 633 nm pump pulse and 658 nm CW probe beam. The absorption saturation followed by a strong absorption of the probe below steady-state transmission level was observed. The recovery of the centers to the original level occurs slowly with ~500 ns time scale and reveals multi-exponential rates with no long-term bleaching or residual absorption. The branching ratio for relaxation process to the ground state and to the metastable state was estimated to be ~ 0.50.
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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.