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Physical review. B, Condensed matter

Cross-relaxation effects in the 2.818-eV zero-phonon emission in brown diamond

Ichiro Hiromitsu, J. Westra, Max Glasbeek

Published Sep 1, 1992• 7 citations
Publisher

Abstract

In brown diamond, the long-lived emission at 2.818 eV is known to be due to a localized center in the photoexcited triplet state. In this paper, the emission intensity of the 2.818-eV center is studied as a function of the strength of an externally applied magnetic field. The cross-relaxation (CR) with N-V centers, ${\mathit{P}}_{1}$ centers, and g=2 doublet spins of unknown origin, as well as level anticrossing (LAC), is found to affect the phosphorescence intensity for certain magnetic-field strengths and orientations. The CR dynamics is studied optically by measuring the phosphorescence transients induced by microwave pulses resonant with a spin transition in the photoexcited triplet state. Under CR conditions, spin population relaxation in the excited triplet state becomes faster and deviates from a single-exponential recovery behavior. The triplet-state kinetics including CR effects is studied theoretically, and a double-exponential recovery is predicted. Based on an analysis of the kinetics, the experimental microwave recovery transients under the CR conditions are satisfactorily simulated. The CR rate is estimated to be (5.0\ifmmode\pm\else\textpm\fi{}1.5)\ifmmode\times\else\texttimes\fi{}${10}^{2}$ ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ for the CR with the N-V center and (8.0\ifmmode\pm\else\textpm\fi{}2.5)\ifmmode\times\else\texttimes\fi{}${10}^{2}$ ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ for the CR with the g=2 doublet species.

DOI
10.1103/physrevb.46.5303

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arXiv:1609.06661•Sep 21, 2016•0 citations
In brown diamond, the long-lived emission at 2.818 eV is known to be due to a localized center in the photoexcited triplet state. In this paper, the emission intensity of the 2.818-eV center is studied as a function of the strength of an externally applied magnetic field. The cross-relaxation (CR) with N-V centers, P1{\mathit{P}}_{1}P1​ centers, and g=2 doublet spins of unknown origin, as well as level anticrossing (LAC), is found to affect the phosphorescence intensity for certain magnetic-field strengths and orientations. The CR dynamics is studied optically by measuring the phosphorescence transients induced by microwave pulses resonant with a spin transition in the photoexcited triplet state. Under CR conditions, spin population relaxation in the excited triplet state becomes faster and deviates from a single-exponential recovery behavior. The triplet-state kinetics including CR effects is studied theoretically, and a double-exponential recovery is predicted. Based on an analysis of the kinetics, the experimental microwave recovery transients under the CR conditions are satisfactorily simulated. The CR rate is estimated to be (5.0\ifmmode\pm\else\textpm\fi{}1.5)\ifmmode\times\else\texttimes\fi{}102{10}^{2}102 s\ensuremath−1{\mathrm{s}}^{\mathrm{\ensuremath{-}}1}s\ensuremath−1 for the CR with the N-V center and (8.0\ifmmode\pm\else\textpm\fi{}2.5)\ifmmode\times\else\texttimes\fi{}102{10}^{2}102 s\ensuremath−1{\mathrm{s}}^{\mathrm{\ensuremath{-}}1}s\ensuremath−1 for the CR with the g=2 doublet species.
Upon the cw optical excitation of N-V centers in diamond, a spin alignment in the ensemble of nonexcited N-V defects in the electron spin-triplet ground state is induced. When the diamond sample is subjected to magnetic fields of suitable directions and strengths, cross relaxation (CR) and level anticrossing are found to affect the ground-state spin alignment as well as the intensity of the emission due to the photoexcited N-V centers. In this paper, a study of the dynamics involved in the cross-relaxation and autocrossing processes is reported, utilizing techniques for the optical detection of spin-coherent transients. A major finding is that when CR conditions prevail, the stimulated spin-echo and spin-locking signals decay at a rate about three times faster than in the situation in which CR does not occur. The results are accounted for by considering the magnetic dipole-dipole interactions within the ensemble of N-V centers in the triplet ground state in a memory function approach.
The spin-selective photokinetics of a single matrix-isolated impurity molecule with a triplet-triplet optical transition, T 0–T 1, is considered and the manifestations of the photokinetics in the fluorescence excitation spectra and intensity autocorrelation functions g (2)(τ) of the molecule undergoing narrow-band optical excitation is studied to resolve the fine structure of the transition. The rates of intersystem crossings (ISCs) T 1→S→T 0 to and from a nonradiating singlet state S of the molecule and the rate of population relaxation among the ground (T 0) state sublevels can be obtained from the spectra and g (2)(τ) using the analytical expressions obtained. New experiments on an individual NV defect center in nanocrystals of diamond, where, for the first time, the fine structure of its triplet-triplet 3 A-3 E zero-phonon optical transition (~637 nm) at 1.4 K was resolved, are interpreted. It is concluded that the rate of the ISC transition from the m S =0 sublevel of the excited 3 E state to the singlet 1 A state (~1 kHz) is much slower than the rates from the m S =±1 substates, while the rates of ISC transitions to different m S substates of the ground 3 A state are close to each other (~1 Hz). As a result, only the optical transition between m S =0 sublevels in the 3 A-3 E manifold contributes strongly to the fluorescence. The experimentally observed double-exponential decay of the g (2)(τ) function is explained by the two pathways available to the center for it to leave the S state: (i) the S→ T 0(m S )=0) transition and (ii) the S→T 0(m S =±1) transitions followed by the slow spin-lattice relaxation T 0(m S =±1)→T 0(m S =0) (rate ~0.1 Hz). The work is important for studies where the NV center is used as a single photon source or for quantum information processing.
Raman-heterodyne-detected paramagnetic resonance has been used to study the level anticrossing in the 3^{3}3A state of the N-V defect in diamond. The electron-paramagnetic-resonance (EPR) frequencies are well accounted for by a triplet-spin Hamiltonian. Comparison of the EPR spectra with the calculated transition dipole strengths indicates that optical pumping determines, to a large extent, the Raman-heterodyne-signal intensity. Spin alignment in the 3^{3}3A ground state under optical pumping leads to the collapse of the EPR signal at the level anticrossing, where the population is equalized due to the mixing of the spin states. This is substantiated by transient nutation and spin-echo measurements, from which the dipole moment and dephasing time are examined. Laser detuning within the 638-nm zero-phonon line shows that the Raman signal is only detectable when the laser frequency is tuned to the low-energy part of the optical line.
We report a study of the magnetic field dependence of the photo-luminescence of NV−^-− centers (negatively charged nitrogen-vacancy centers) in diamond single crystals. In such a magnetic field dependence characteristic lines are observed, which are coming from Level Anti-Crossings (LACs) in the coupled electron-nuclear spin system. For enhancing the sensitivity, we used lock-in detection to measure the photo-luminescence intensity and observed a remarkably strong dependence of the LAC-derived lines on the modulation frequency. Upon decreasing of the modulation frequency from 12 kHz to 17 Hz the amplitude of the lines increases by approximately two orders of magnitude. To take a quantitative account for such effects, we developed a theoretical model, which describes the spin dynamics in the coupled electron-nuclear spin system under the action of an oscillating external magnetic field. Good agreement between experiments and theory allows us to conclude that the observed effects are originating from coherent spin polarization exchange in the NV−^-− center. Our results are of great practical importance allowing one to optimize the experimental conditions for probing LAC-derived lines in diamond defect centers.