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Bulletin of the Lebedev Physics Institute

Spectral and Temporal Characteristics of Narrowband Superluminescence of NV– and C Centers in High-Pressure High-Temperature Diamond

V.F. Lebedev, T.S. Misnikova, Ya. A. Ryvkina, E. A. Vasil’ev, I. V. Klepikov, A. V. Koliadin, Victor G. Vins

Published Dec 1, 2025• 0 citations
Publisher

Abstract

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.

DOI
10.3103/s1068335625604819

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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.
Abstract We report an investigation of spectral and temporal properties of NV¯ centers in diamond plates fabricated from a single HPHT crystal but subjected to different electron irradiation doses during postgrowth processing. Samples 52734-1 and 52734-2, each with approximately the same nitrogen concentration of 60 ppm, are irradiated with doses of 1 and 2 × 1018 e‒/cm2, respectively. Particular attention is paid to the effect of irradiation dose on the concentration of NV¯ centers and the associated changes in the spectral and temporal properties of superluminescence under identical conditions of optical excitation with laser radiation at a wavelength of 532 nm. Analysis of the absorption spectra reveals that doubling the irradiation dose results in a 1.4-fold increase in the concentration of NV¯ centers—from 7.7 to 10.9 ppm—with a corresponding decrease in the concentration of isolated nitrogen centers (C centers)—from 49 to 43 ppm. The results demonstrate a nonlinear dependence of the increase in the concentration of NV¯ centers on the irradiation dose and make it possible to identify key characteristics of the samples and pumping conditions that determine the efficiency of superluminescence. Specifically, doubling the irradiation dose results in a threefold increase in the spectral intensity and a significant decrease in the duration of the superluminescence pulses. It is found that to achieve efficient superluminescence, it is important not only to have a significant excess of the concentration of C centers over the concentration of NV¯ centers, but also the absolute concentration of NV¯ centers and pump parameters such as the energy density of the pump pulses and the volume of the sample with a population inversion.
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 In the context of the NV− diamond laser creation [1], an urgent task is to determine the characteristics of diamonds that can affect the laser generation. This work is aimed at investigating the mechanisms of the creation of superluminescence in diamond under the action of optical pumping by the second harmonic of the Nd:YAG laser (λ = 532nm). It was found that when the HPHT diamond is irradiated by 532 nm radiation with an intensity above ~ 2.0 MW/cm2, a nonlinear intensity increasing in the spectral region 700–750 nm is manifested against the background of the spontaneous photoluminescence spectrum, which, with a further pumping intensity increasing turns into a pronounced peak of superluminescence with a maximum of about 718 nm. An increase in the pumping intensity from 2.7 to 46 MW/cm2 widened this peak at half-maximum from 13 to 19 nm. At high levels of pumping intensity, nonlinear pumping radiation absorption and accumulation of NV centers in the excited state were detected. The position of the photoluminescence band was calculated depending on different values of the population inversion density of the color centers, taking into account the diamond's own absorption spectrum. The calculation results are close to the experimental data.
Abstract Superluminescence of NV centres with a band peaking at λ = 718 nm in the phonon wing of the photoluminescence spectrum of a high-pressure high-temperature (HPHT) diamond sample under pulsed optical excitation at λ = 532 nm with an intensity of 2 – 46 MW cm−2 is demonstrated. Superluminescence is observed in the diamond crystal region containing 6 ppm NV centres and 150 ppm substituent nitrogen; it is absent in the crystal part with a lower nitrogen content. Superluminescence pulses are observed on the leading edge of the optical excitation pulse at λ = 532 nm and have an FWHM value of 4 ns. The enhancement of the photoluminescence of NV centres is suggested to be due to the total internal reflection in the diamond plate (waveguide effect).
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.
In the light of the creation of a diamond laser [1], an urgent task is to determine the characteristics of diamonds in order to determine the range in which such lasers can be created not in isolated cases. This work is aimed at studying the mechanisms of creating superluminescence in diamond under the action of optical pumping by the second harmonic of an ND:YAG laser (λ = 532 nm). It was found that, upon pulsed excitation of a diamond by an ND:YAG laser with a pump intensity above ~2.0 MW/cm2 in the spectral range 700–750 nm, a nonlinear increase in intensity appears against the background of the spontaneous photoluminescence spectrum, which, with a further increase in the pump intensity, turns into a pronounced superluminescence peak with a maximum at about 718 nm. An increase in the pump intensity from 2.7 to 46 MW/cm2leads to the broadening of this peak at half maximum from 13 to 19 nm. At high levels of pump intensity, nonlinear absorption of pump radiation and accumulation of NV centers in the excited state were found. The position of the photoluminescence band was calculated as a function of various values of the inversion density of the populations of color centers, taking into account the intrinsic absorption spectrum of diamond. The calculation results are close to the experimental data.