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Information-measuring and Control Systems

Analysis of spectral and temporal characteristics of stimulated emission of HPHT-diamonds with nitrogen-vacancy - colouring centres

T.S. Misnikova

Published Jan 1, 2025• 1 citation
Publisher

Abstract

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.

DOI
10.18127/j20700814-202504-08

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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.
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.
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.
In this paper, a brief overview of the main characteristics of lasers at NV centers in diamond is carried out. Currently, lasers at NV centers in a negative charge state generate pulsed laser radiation in the range of 714-720 nanometers with a duration of units of nanoseconds with a pulse energy of tens of microjoules and an efficiency of several percent. A significant increase in the efficiency and energy characteristics of NV lasers can be achieved through the use of multilayer reflective coatings on the faces of crystals as resonator mirrors. Lasers of this class have good prospects in the field of obtaining femtosecond pulses, since NV centers have a wide luminescence contour. Due to the high thermal conductivity of the diamond, they are able to provide generation with a high level of average power. To increase the pulse duration and transition to continuous generation, it is necessary to pump with a high level of average power. A possible solution would be injection pumping. This requires the creation of efficient light-emitting diamond electroconductive structures. In addition, the article presents new data on the study of spectral characteristics of the superluminescence of the NV centers of a diamond laser when the crystal is heated from 100 to 300 K. It is shown that the superluminescence band of such lasers actually consists of two spectral components that are not resolved at room temperature. The temperature behavior of these components is fundamentally different: the short-wave component practically does not change in intensity, while the long-wave component exponentially increases in intensity to 220 K, and then saturates and further decreases according to Mott's law. In addition, it was found that the maxima of these components experience a shift in the long-wavelength direction by about 6 meV when the temperature changes from 100 to 300 K. In the future, it is necessary to find out the exact nature and physical mechanisms of the detected phenomena, as well as to find their possible practical applications. The authors declare no conflicts of interests.
Stimulated emission is the process fundamental to laser operation, thereby producing coherent photon output. Despite negatively charged nitrogen-vacancy (NV−) centres being discussed as a potential laser medium since the 1980s, there have been no definitive observations of stimulated emission from ensembles of NV− to date. Here we show both theoretical and experimental evidence for stimulated emission from NV− using light in the phonon sidebands around 700 nm. Furthermore, we show the transition from stimulated emission to photoionization as the stimulating laser wavelength is reduced from 700 to 620 nm. While lasing at the zero-phonon line is suppressed by ionization, our results open the possibility of diamond lasers based on NV− centres, tuneable over the phonon sideband. This broadens the applications of NV− magnetometers from single centre nanoscale sensors to a new generation of ultra-precise ensemble laser sensors, which exploit the contrast and signal amplification of a lasing system. Here Jeskeet al. show both theoretical and experimental evidence for stimulated emission from negatively charged nitrogen vacancy centres using light in the phonon sidebands around 700 nm, demonstrating its suitability as a laser medium.