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Optics Letters

Visible color-center laser in diamond

Stephen Colby Rand, L. G. DeShazer

Published Oct 1, 1985• 100 citations
Publisher

Abstract

Laser action at 530 nm using H3 centers in diamond was observed with an efficiency of 13.5% at room temperature. Optical double-resonance experiments on N3 centers provided direct evidence for a (2)A metastable level. Its presence results in rapid decay of the excited (2)E state and low quantum efficiency as well as significant excited-state absorption in the N3 luminescence region.

DOI
10.1364/ol.10.000481

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•Mar 9, 2022•0 citations
Laser action at 530 nm using H3 centers in diamond was observed with an efficiency of 13.5% at room temperature. Optical double-resonance experiments on N3 centers provided direct evidence for a (2)A metastable level. Its presence results in rapid decay of the excited (2)E state and low quantum efficiency as well as significant excited-state absorption in the N3 luminescence region.
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%.
We report the observation of cw four-wave mixing and phase conjugation in the UV on the N3 color-center resonance in diamond. Using a jitter-free technique, the nearly degenerate four-wave mixing spectrum has been measured and the ultranarrow, 250-Hz-wide resonance analyzed to understand the metastable-state decay process responsible for the low quantum efficiency and large nonlinear susceptibility of this aggregated nitrogen structure. The results establish the existence and lifetime of a new excited state of the defect.
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.
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.
This review analyzes theoretical calculations and laboratory experiments showing the prospects of using of diamond with color centers as active laser medium. Despite the mentioned prospects, practical implementation of lasers based on color centers in diamond is limited to laboratory demonstrations. No commercially significant products of laser technology based on diamond with color centers have been created yet. Obviously, the available scientific information is still insufficient, and additional research is required. The review analyzes the factors that require further study: concentration quenching of luminescence, thermal quenching of luminescence, luminescence quenching by nitrogen and other impurity defects, as well as the influence of multiphoton and multi-stage absorption processes. For color centers in diamond, such processes have yet to be investigated in more detail.
The H3 center in diamond has been shown to exhibit several promising characteristics for laser cooling applications including a neutral charge state, high radiative quantum yield, and efficient anti-Stokes photoluminescence. In this work, we show that upon excitation with a 532 nm laser, bulk diamond crystals doped with H3 centers emit efficient up-conversion photoluminescence and also show significantly reduced photothermal heating relative to crystals doped with NV centers. These results encourage future exploration of techniques for H3 enrichment in diamonds at high-pressure, high-temperature conditions for the simultaneous anti-Stokes fluorescence cooling and radiation balanced lasing in semiconductor materials.