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Journal of Experimental and Theoretical Physics Letters

One-Photon Femtosecond Laser Excitation of Photoluminescence from H3 and H4 Centers in Natural Diamond: A Method to Determine Their Concentration

Sergey Ivanovich Kudryashov, П. А. Данилов, Victor G. Vins, Daniil A. Pomazkin, P. P. Pakholchuk, М. Л. Скориков, Igor V. Smetanin, Pham Van Duong, Pham Hong Minh

Published Feb 1, 2024• 4 citations
Publisher

Abstract

The photoluminescence spectra of the dominant H3 and H4 centers in a natural diamond sample, which is preliminarily characterized by optical and infrared spectrophotometry, are excited by femtosecond laser pulses with a wavelength of 470 nm and varying intensity. Saturation of the photoluminescence intensity of the H3 and H4 centers normalized by the intensity of laser radiation is observed and attributed to the saturation of the resonance transition responsible for the excitation. This makes it possible for the first time to estimate the absorption cross sections of H3 and H4 centers, which can be compared with values known from the literature and those determined from photoluminescence kinetics. The total concentration of H3 and H4 centers can then be found. Taking into account the known absorption coefficient of the sample at a wavelength of 470 nm and the previously established ratio of the contributions from H3 and H4 centers, their concentrations have been estimated separately for the first time.

DOI
10.1134/s0021364022601312

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The photoluminescence spectra of the dominant H3 and H4 centers in a natural diamond sample, which is preliminarily characterized by optical and infrared spectrophotometry, are excited by femtosecond laser pulses with a wavelength of 470 nm and varying intensity. Saturation of the photoluminescence intensity of the H3 and H4 centers normalized by the intensity of laser radiation is observed and attributed to the saturation of the resonance transition responsible for the excitation. This makes it possible for the first time to estimate the absorption cross sections of H3 and H4 centers, which can be compared with values known from the literature and those determined from photoluminescence kinetics. The total concentration of H3 and H4 centers can then be found. Taking into account the known absorption coefficient of the sample at a wavelength of 470 nm and the previously established ratio of the contributions from H3 and H4 centers, their concentrations have been estimated separately for the first time.
In this work, we focus on the interaction of SiV color centers in diamond with femtose- cond light pulses. In the theoretical part, a script is developed to simulate the experimen- tal varying stripe length method and the effects of saturated optical gain are investigated. In the experimental part, photoluminescence and transient differential absorption under non-resonant excitation are studied. The result of the luminescence measurements are estimates of the effective cross-sections of single-photon absorption for the wavelengths 620 nm, 515 nm and 340 nm, as well as the effective cross-section of three-photon absorp- tion for 2000 nm. The result of the differential absorption measurements is the relaxation constant of the excited level of the SiV center and the upper estimate of the time duration of the initial dynamics. 1
In this work, we focus on the interaction of SiV color centers in diamond with femtose- cond light pulses. In the theoretical part, a script is developed to simulate the experimen- tal varying stripe length method and the effects of saturated optical gain are investigated. In the experimental part, photoluminescence and transient differential absorption under non-resonant excitation are studied. The result of the luminescence measurements are estimates of the effective cross-sections of single-photon absorption for the wavelengths 620 nm, 515 nm and 340 nm, as well as the effective cross-section of three-photon absorp- tion for 2000 nm. The result of the differential absorption measurements is the relaxation constant of the excited level of the SiV center and the upper estimate of the time duration of the initial dynamics. 1
Nonlinear optical absorption in commercially available diamond crystals containing nitrogen-vacancy (NV) centers is investigated using femtosecond open-aperture Z-scan measurements at a wavelength of 1032 nm. Experiments were performed on a high-purity electronic-grade diamond and on samples with moderate and high NV concentrations. While the undoped crystal exhibits third-order nonlinear absorption, the NV-doped samples show a pronounced saturable absorption response. To elucidate the microscopic origin of this effect, the Z-scan results are analysed in conjunction with linear transmission spectra, which reveal the presence of additional nitrogen-related defect complexes, including H2 ( NVN−\hbox {NVN}^{-}NVN− ) centers. Although the excitation wavelength is detuned from the principal zero-phonon lines of both NV and H2 defects, it overlaps with the broader near-infrared absorption band associated with vibronic transitions. A quantitative analysis based on an effective two-level model indicates that the observed saturable absorption is most consistently explained by a dominant contribution from H2 defects, while a weaker off-resonant contribution from NV centers cannot be excluded. The extracted parameters, including the linear absorption coefficient and saturation intensity, are supported by a reconstruction of the defect-related absorbance spectrum and by consistency with previously reported nonlinear refractive index data. These results highlight the importance of complex defect environments in determining the nonlinear optical response of NV-doped diamond and provide insight into defect-specific contributions relevant for diamond-based nonlinear and quantum photonic applications.
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.
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.
Color centers in diamond have a potential for opto-electronic applications. Laser action of H3 centers in natural diamond has been already reported. Our interest is focused on the possibility of laser action using synthetic diamond. A first attempt was made to produce H3 centers with high density in synthetic diamond. Optical properties of the H3 centers were investigated. Sample-dependent luminescence decay time and long lived transient absorption were observed. Laser action using the H3 centers in synthetic diamond occurred though the efficiency was as low as 0.1%.