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Journal of The Electrochemical Society

Phosphorescence Polarization and Coherence of the 2.818 eV Center in Diamond

Max Glasbeek, Ichiro Hiromitsu, J. Westra

Published May 1, 1993• 1 citation
Publisher

Abstract

The polarization properties of the sublevel emission from the phosphorescent triplet state of the 2.818 eV center in diamond have been investigated. Furthermore, optically detected spin coherent transients have been studied for the photoexcited state of the 2.818 eV center at 1.4 K. Dynamical magnetic dipole‐dipole interactions with flipping electron spins at nearby lattice sites induce dephasing and spectral diffusion.

DOI
10.1149/1.2221568

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

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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.

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The polarization properties of the sublevel emission from the phosphorescent triplet state of the 2.818 eV center in diamond have been investigated. Furthermore, optically detected spin coherent transients have been studied for the photoexcited state of the 2.818 eV center at 1.4 K. Dynamical magnetic dipole‐dipole interactions with flipping electron spins at nearby lattice sites induce dephasing and spectral diffusion.
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 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ for the CR with the N-V center and (8.0\ifmmode\pm\else\textpm\fi{}2.5)\ifmmode\times\else\texttimes\fi{}102{10}^{2}102 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ 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.
Quantum-beat spectroscopy has been used to observe excited states of the N-V center in diamond. For the 1.945-eV optical transition, direct evidence is presented for the existence of GHz-scale fine structure, together with a much larger 46-${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ level splitting in the E state. An interference effect observed in transient four-wave-mixing response is explained with a polarization selection rule involving Zeeman coherence among magnetic sublevels. Also, detailed dephasing measurements versus temperature and wavelength have identified the decay mechanisms operative among the various states. A comparison of these results with ab initio calculations of excited electronic structure and interactions based on several multielectron models supports the conclusion that the N-V center is a neutral, two-electron center governed by a strong Jahn-Teller effect and weak spin-spin interactions. \textcopyright{} 1996 The American Physical Society.
Color centers in diamond are a promising platform for quantum communication, as they can serve as solid state quantum memories with efficient optical transitions. Much recent attention has focused on the negatively charged NV center in diamond, which has a spin triplet ground state electronic configuration that can be measured and initialized optically, exhibits long spin coherence times at room temperature, and has narrow, spin-conserving optical transitions. However, the NV center exhibits a large static and dynamic inhomogeneous linewidth, and over 97% of its emission is in a broad, incoherent phonon side band, severely limiting scalability. Alternatively, the negatively charged SiV center exhibits excellent optical properties, with 70% of its emission in the zero phonon line and a narrow inhomogeneous linewidth. However, SiV− suffers from short electron spin coherence times, limited by an orbital relaxation rate (T1) of around 40 ns at 5 K.
A lead-vacancy (PbV) center in diamond exhibits coherent emission above the liquid helium temperature, making it highly attractive for quantum network applications. Here, we report the magneto-optical and spin properties of PbV centers in diamond. We record a spin lifetime of 12 ms at 7.5 K under large off-axis magnetic field. Furthermore, we observe formation of the coherent dark state by coherent population trapping and estimate a spin dephasing time of 177 ns at 6.5 K. This work demonstrates the outstanding thermal robustness of the PbV spin compared to other group-IV centers above 4 K.