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Journal of Physics C Solid State Physics

Resonant excitation of the GR centre in diamond

Alan T. Collins, J Szechi, Susan M. Tavender

Published Mar 10, 1988• 29 citations
Publisher

Abstract

Photoluminescence in the GR1 zero-phonon region has been examined in detail, using a tunable dye laser resonant with the higher excited states GR2 to GR8. The authors conclude that the temperature-dependent structure observed when electron beam excitation is used is not due to perturbation of the centre resulting from the fast non-radiative relaxation from the higher levels to the first excited state.

DOI
10.1088/0022-3719/21/7/001

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Journal of Physics C Solid State Physics•Mar 20, 1984•64 citations
Photoluminescence in the GR1 zero-phonon region has been examined in detail, using a tunable dye laser resonant with the higher excited states GR2 to GR8. The authors conclude that the temperature-dependent structure observed when electron beam excitation is used is not due to perturbation of the centre resulting from the fast non-radiative relaxation from the higher levels to the first excited state.
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.
Color centers in diamond are important quantum emitters for a broad range of applications ranging from quantum sensing to quantum optics. Understanding the internal energy level structure is of fundamental importance for future applications. We experimentally investigate the level structure of an ensemble of few negatively charged silicon-vacancy (SiV − ) and germanium-vacancy (GeV − ) centers in bulk diamond at room temperature by photoluminescence (PL) and excitation (PLE) spectroscopy over a broad wavelength range from 460 to and perform power-dependent saturation measurements. For SiV − our experimental results confirm the presence of a higher energy transition at . By comparison with detailed theoretical simulations of the imaginary dielectric function we interpret the transition as a dipole-allowed transition from -state to -state where the corresponding a 2 u -level lies deeply inside the diamond valence band. Therefore, the transition is broadened by the diamond band. At higher excitation power of we indicate signs of a parity-conserving transition at supported by saturation measurements. For GeV − we demonstrate that the PLE spectrum is in good agreement with the mirror image of the PL spectrum of the zero-phonon line. Experimentally we do not observe a higher lying energy level up to a transition wavelength of . The observed PL spectra are identical, independent of excitation wavelength, suggesting a rapid decay to excited state and followed by optical transition to ground state. Our investigations convey important insights for future quantum optics and quantum sensing experiments based on SiV − -center and GeV − -center in diamond.
We study the decay kinetics of excited state of GR1 center in diamond using 633 nm pump pulse and 658 nm CW probe beam. The absorption saturation followed by a strong absorption of the probe below steady-state transmission level was observed. The recovery of the centers to the original level occurs slowly with ~500 ns time scale and reveals multi-exponential rates with no long-term bleaching or residual absorption. The branching ratio for relaxation process to the ground state and to the metastable state was estimated to be ~ 0.50.
We report the photoluminescence characteristics of a colour centre in diamond grown by plasma-assisted chemical vapour deposition. The colour centre emits with a sharp zero-phonon line at 2.330 eV (λ=532 nm) and a lifetime of 3.3 ns, thus offering potential for a high-speed single-photon source with green emission. It displays a vibronic emission spectrum with a Huang–Rhys parameter of 2.48 at 77 K. Hanbury–Brown and Twiss measurements reveal that the electronic level structure of the defect includes a metastable state that can be populated from the optically excited state.
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).