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Properties of color centers in diamond studied by methods of femtosecond laser spectroscopy

Neli Streshkova

Published Jan 1, 2022• 0 citations
OpenAlex

Abstract

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

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Properties of color centers in diamond studied by methods of femtosecond laser spectroscopy

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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

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

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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.

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Single crystal diamonds with strong NV− luminescence were prepared by high-pressure high-temperature method and followed by electron irradiation and annealing process. The stimulated emission and gain characteristics of NV− diamond in femtosecond time scale are also studied using the transient absorption technique. Stimulated emission was observed at 660–800 nm, with an optical gain displayed in the range of 680–725 nm. Further test revealed that the optical gain lifetime is 3.5 ns and the gain coefficient is 0.16 cm−1, demonstrating the potential realization of color center lasers.

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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.

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Fluorescence dynamics of color centers in diamond needles

Филоненко Елена Михайловна, P. Kuzhir, Sergei Malykhin

Abstract This study presents a detailed investigation into the fluorescence properties of color centers in single-crystal diamond needles (SCDNs) synthesized via chemical vapor deposition. Using steady-state and time-resolved photoluminescence (PL) techniques, we identified color centers with zero-phonon lines at 389 nm, 468 nm, 575 nm (NV0), 637 nm (NV–), and 738 nm (SiV–). PL excitation spectroscopy conducted at room temperature revealed the complex electronic structure of some of these centers, paving the way for further investigation into their fluorescence properties. Lifetime measurements were performed for each center, with the 389 nm one exhibiting the longest decay time (∼30 ns), which is advantageous for enhancing quantum coherence, improving photon emission efficiency, and reducing power consumption. Altogether, these findings highlight the potential of SCDNs for quantum applications and confirm their promise as a platform for next-generation photonic and quantum devices.

Nanotechnology•Mar 25, 2025•1 citation

Spectroscopy of GR1 centers in synthetic diamonds

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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.

Optical Materials Express•Feb 12, 2021•20 citations
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
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.
Single crystal diamonds with strong NV− luminescence were prepared by high-pressure high-temperature method and followed by electron irradiation and annealing process. The stimulated emission and gain characteristics of NV− diamond in femtosecond time scale are also studied using the transient absorption technique. Stimulated emission was observed at 660–800 nm, with an optical gain displayed in the range of 680–725 nm. Further test revealed that the optical gain lifetime is 3.5 ns and the gain coefficient is 0.16 cm−1, demonstrating the potential realization of color center lasers.
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.
Abstract This study presents a detailed investigation into the fluorescence properties of color centers in single-crystal diamond needles (SCDNs) synthesized via chemical vapor deposition. Using steady-state and time-resolved photoluminescence (PL) techniques, we identified color centers with zero-phonon lines at 389 nm, 468 nm, 575 nm (NV0), 637 nm (NV–), and 738 nm (SiV–). PL excitation spectroscopy conducted at room temperature revealed the complex electronic structure of some of these centers, paving the way for further investigation into their fluorescence properties. Lifetime measurements were performed for each center, with the 389 nm one exhibiting the longest decay time (∼30 ns), which is advantageous for enhancing quantum coherence, improving photon emission efficiency, and reducing power consumption. Altogether, these findings highlight the potential of SCDNs for quantum applications and confirm their promise as a platform for next-generation photonic and quantum devices.
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.