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Journal of Physics C Solid State Physics

Persistent spectral hole burning of colour centres in diamond

Richard T. Harley, M J Henderson, R. M. Macfarlane

Published Mar 20, 1984• 64 citations
Publisher

Abstract

Four zero-phonon lines of defect centres in diamond (GR1 (741 nm), N-V (637 nm), H4 (496 nm) and N3 (415 nm)) have been shown to exhibit persistent spectral hole burning. The phenomenon appears to be a rather general one in diamond and should prove very powerful for elucidation of the nature of defect centres. As an example, preliminary results for the N-V centre suggest a previously undetected splitting of the excited state.

DOI
10.1088/0022-3719/17/8/002

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Four zero-phonon lines of defect centres in diamond (GR1 (741 nm), N-V (637 nm), H4 (496 nm) and N3 (415 nm)) have been shown to exhibit persistent spectral hole burning. The phenomenon appears to be a rather general one in diamond and should prove very powerful for elucidation of the nature of defect centres. As an example, preliminary results for the N-V centre suggest a previously undetected splitting of the excited state.
In this paper an overview on the spectroscopic and spectral hole-burning properties of radiation-induced spectral lines in nitrogen-containing diamonds is given. Special attention has been paid to the defects with the 774 and 813 nm zero-phonon lines that are suitable for room temperature spectral hole burning. The temperature dependence of the widths of the homogeneous lines is carefully examined. Persistent spectral hole burning in these lines is demonstrated at T = 100, 200 and 300 K. The creation of these colour centres dependent on irradiation and annealing parameters in different types of diamonds is investigated. Assumptions about the nitrogen content of the centres are made on the basis of these investigations. The possibility of producing the 774 and 813 nm centres in synthetic diamonds is shown and the optimal parameters are given.
In this presentation we report on several spectral features associated with Si impurity in diamond related to spectral hole-burning. Diamond, with its hardness and high temperature stability, is a potentially useful material for high temperature hole-burning storage. The first hole-burning in bulk diamonds [1] was observed from color centers in the spectra of N3 at 415 nm, H4 at 496 nm, N-V at 637 nm, and GR1 at 741 nm. Recently, hole-burning was observed for color centers N-V at 637 nm and 574 nm of electron irradiated chemical-vapor deposited (CVD) diamonds [2].
A persistent spectral hole-burning technique has been employed to investigate the impact of uniaxial stress on the defects created by neutron irradiation in natural Ia-type diamond. Shifts of the spectral holes in the 649, 681, and 774 nm zero-phonon lines (ZPLs) have been measured. The values of the shifts, 2.2, 1.2, and 0.65 cm−1/kbar, obtained from these measurements have been compared with the stress shifts of the lines of defects with well-known structure. It is suggested that vacancies are present in the defect responsible for the 681 nm ZPL. A combination of the results of polarized luminescence and uniaxial stress experiments leads to the conclusion of rhombic I symmetry of the defects that give rise to the 649 and 681 nm ZPLs.
The persistent spectral hole burning effect has been observed for the nitrogen vacancy (NV) center and the 2.16 eV center in chemical-vapor deposited (CVD) diamond. This sideband is the first observation of spectral hole burning in CVD diamond. Holes are burned in the inhomogeneously broadened zero-phonon lines of both the centers by dye lasers. The holes were observed by photoluminescence excitation spectroscopy, with monitoring of the phonon-sideband emission, at temperatures up to 130 K for the NV center and up to 100 K for the 2.16 eV center.
New satellite features and antiholes in the persistent hole-burning spectrum of N–V centers in diamond, as well as their dependences on applied electric fields and frequency within the inhomogeneous absorption line, are reported. These results, together with reassignments of spin states of this center, permit an understanding of the origin of the satellite holes as well as of possible mechanisms for the persistent hole-burning phenomenon itself. In addition we report narrow optical interference fringes in heterodyne-detected spectra of persistent spectral holes in the N–V defect center in diamond and discuss a recent suggestion for high-resolution Ramsey-fringe hole-burning spectroscopy of solids based on phase-separated fields.
With a ring dye laser persistent spectral hole-burning was measured by fluorescence excitation spectroscopy in the zero-phonon lines of the 2llg ↔ 2llu transition in KI:S2 − and of the 3H4 → 3P0 transition of a defect center with three D− ions in SrF2:Pr3+:D−and also in the zero-phonon line at 462.5 nm of a color center in neutron-irradiated and annealed α-Al2O3. In all three lines holes with a width in the order of 1 GHz could be obtained at 1.5 K with single frequency laser. With broad-band laser in KI:S2 − and SrF2:Pr3+:D− spectral redistribution within the full range of inhomogeneous broadening could be observed which are explained by a photophysical model based on barrier crossing in asymmetric double-well-potentials. In the case of sapphire a photobleaching process is dominant which is effective also for nonselective excitation, and the holes are thermoresistant up to 300 K.