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Optics Letters

Two-beam coupling by nitrogen-vacancy centers in diamond

David A. Redman, Q. Z. Shu, Alan Lenef, S. C. Rand

Published Feb 1, 1992• 14 citations
Publisher

Abstract

A new method for two-beam coupling measurements based on acousto-optic modulation with subhertz tuning capability is applied to study excited-state dynamics of the nitrogen-vacancy center in diamond. Results yield fundamental decay constants and the nonlinear refractive index and are in good agreement with the calculated dual grating response to resonances in the microscopic susceptibility due to intersystem crossing and spin-lattice relaxation.

DOI
10.1364/ol.17.000175

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A new method for two-beam coupling measurements based on acousto-optic modulation with subhertz tuning capability is applied to study excited-state dynamics of the nitrogen-vacancy center in diamond. Results yield fundamental decay constants and the nonlinear refractive index and are in good agreement with the calculated dual grating response to resonances in the microscopic susceptibility due to intersystem crossing and spin-lattice relaxation.
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We investigate spin-dependent decay and intersystem crossing (ISC) in the optical cycle of single negatively charged nitrogen-vacancy (NV) centres in diamond. We use spin control and pulsed optical excitation to extract both the spin-resolved lifetimes of the excited states and the degree of optically induced spin polarization. By optically exciting the centre with a series of picosecond pulses, we determine the spin-flip probabilities per optical cycle, as well as the spin-dependent probability for ISC. This information, together with the independently measured decay rate of singlet population, provides a full description of spin dynamics in the optical cycle of NV centres. The temperature dependence of the singlet population decay rate provides information about the number of singlet states involved in the optical cycle.