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International Conference Laser Optics (ICLO)

Direct observation of stimulated emission of NV– centers in synthetic HPHT diamond

Vyacheslav F. Lebedev, T.S. Misnikova, Ya. A. Ryvkina, D. E. Genin, Andrey V. Samolov, E. I. Lipatov, V.G. Vince, I.V. Klepikov, A. V. Koliadin, R.V. Isakov

Published Jul 1, 2024• 0 citations
Publisher

Abstract

Data on direct observation of stimulated emission of $\mathrm{NV}^{-}$centres in synthetic NRNT-diamonds located in a focused pump beam are presented. The spectra and pulse durations of the stimulated emission were simultaneously recorded. It was found that the shapes of the spectra and the intensity of stimulated emission depend on the number of emitting centres and the position of the crystal relative to the focus of the pump beam.

DOI
10.1109/iclo59702.2024.10624416

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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.

SPIE Solid State Lasers: Technology and Devices•Feb 20, 2018•8 citations
Data on direct observation of stimulated emission of NV−\mathrm{NV}^{-}NV−centres in synthetic NRNT-diamonds located in a focused pump beam are presented. The spectra and pulse durations of the stimulated emission were simultaneously recorded. It was found that the shapes of the spectra and the intensity of stimulated emission depend on the number of emitting centres and the position of the crystal relative to the focus of the pump beam.
Currently, the development of active laser materials is a promising direction, but diamond has not yet been applied in this field. Therefore, one of the most significant advances in diamond physics is stimulated emission (SE) and pulsed laser generation in the spectral range between 710 and 720 nm (1.72-1.74 eV). The presented work shows new experimental data on the spectral and temporal characteristics of stimulated emission produced at nitrogen-vacancy NV -centres (nitrogen-negatively charged vacancy centre) for single-sector {111} HPHT diamond. For this purpose, an experimental bench was developed to obtain spectral and temporal characteristics of the stimulated emission and experiments were carried out. As a result of the analysis of experimental data it was found that in the spectral range of 650-750 nm at excitation by laser radiation with λ=532 nm a rather narrow band of stimulated emission in the region of 705-730 nm with a maximum around 716 nm is emitted. It is demonstrated that there is some dependence of the shapes of spectra and pulses of radiation. It was found that a decrease in pumping energy and irradiation volumes of diamond leads to the appearance of mode structures on the spectrum and peak structures on the oscillogram, and an increase in the spectrum and oscillogram smoothing. However, when the pumping energy is maintained but the irradiation volumes are reduced, the smooth shape of spectra and pulses is preserved. At the same time, the intensity of the spectrum decreases and the duration of the irradiation pulse decreases. Previously, laser generation was obtained on this diamond sample, but it was not achieved in the present work. The reasons for this phenomenon are not clear yet and require additional experiments and analysis of the obtained results.
Abstract— A comparative analysis has been made of the superluminescence spectra of two HPHT diamond samples with NV¯-centers with the concentration in the growth sectors {111} of NV¯-centers ≈10 ppm and of C-centers ≈ 45 ppm. A broad structureless superluminescence band with a maximum about 706 nm and a narrow band in the region of 705 to 720 nm were identified in the spectral range of 650–750 nm when excited by pulsed laser radiation at λ = 532 nm. It was found that the narrow-band superluminescence was not excited by pumping with continuous radiation at λ = 532 nm and the intensities of both types of superluminescence were summated under simultaneous pumping by continuous and pulsed radiation at λ = 532 nm. These data indicate either the different nature of the two types of superluminescence or that they belonged to NV¯ centers but with different excitation mechanisms. The existence of connection between the shape of the spectra of narrow-band superluminescence and of radiation pulses has been demonstrated. The observed features of narrow-band superluminescence are explained for the first time by the occurrence of mode-locking laser generation. The mode-locking laser generation without the use of reflective coatings on the sample or an external resonator on other laser materials has not been observed before.
Abstract We report a study of narrowband superluminescence of a single-sector {111} high-pressure high-temperature (HPHT) diamond plate with NV– and C centers at a total nitrogen and NV– center concentrations of ~60 ppm and 11 ppm, respectively. The sample is optically pumped with pulsed laser radiation (λ = 532 nm) focused by a cylindrical lens (f = 60 mm). It is found that, in the region of the pump beam waist, the superluminescence spectra exhibit a pronounced fine structure, while the radiation pulse has a spike shape with an exponential decrease in pulse intensity over time. With additional pumping with continuous radiation at λ = 403 nm, an increase in the superluminescence intensity is recorded, and the number of intense peaks in the radiation pulse also increases. As the volume of the sample with a population inversion gradually increases by moving it away from the pump beam waist, the superluminescence intensity increases steadily, accompanied by spectrum smoothing, reaching a maximum at approximately a twofold increase in the pump volume. It is found that, with a smooth narrowband superluminescence spectrum, a short single pulse is generated as the narrowband superluminescence intensity approaches saturation.
The photoluminescence spectra of two synthetic diamond samples containing 1-10 ppm NV centers and 100-200 ppm substitutional nitrogen were studied under optical pumping at 532, 560, and 575 nm. At pump intensities less than 0.5-1.0 MW/cm2, a vibronic photoluminescence band of NV- centers in the negative charge state was observed. With an increase in the pump intensity above 0.5-1.0 MW/cm2, a superluminescence band was observed on the long-wavelength shoulder of the phonon wing in the range 700-760 nm. The intensity of superluminescence band increased with increasing pump intensity. It is shown that the position of the superluminescence band with maxima in the range 715-720 nm is unchanged at all of optical pump wavelengths.
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.