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arXiv:1412.4865 · Physical Review B

State-selective intersystem crossing in nitrogen-vacancy centers

Michael Goldman, Marcus W. Doherty, Alp Sipahigil, Norman Y. Yao, Steven D. Bennett, Neil B. Manson, Alexander Kubanek, Mikhail D. Lukin

Published Apr 8, 2015• 151 citations
arXivHTMLPDF

Abstract

Motivated by recent measurements of state-selective intersystem crossing (ISC) in the nitrogen-vacancy (NV) center in diamond (see companion PRL), a new microscopic model is developed of the key ISC mechanism. These nonradiative transitions between states of different spin multiplicity are pivotal in the optical initialization and readout of the NV center's electronic spin, which has created a diverse range of room-temperature applications in metrology and quantum information science.

DOI
10.1103/physrevb.91.165201

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Motivated by recent measurements of state-selective intersystem crossing (ISC) in the nitrogen-vacancy (NV) center in diamond (see companion PRL), a new microscopic model is developed of the key ISC mechanism. These nonradiative transitions between states of different spin multiplicity are pivotal in the optical initialization and readout of the NV center's electronic spin, which has created a diverse range of room-temperature applications in metrology and quantum information science.
The nitrogen-vacancy (NV) center in diamond has emerged as a versatile atom-like system, finding diverse applications at both ambient and cryogenic temperatures. At room temperature, the NV center's spin-triplet electronic ground state has a long coherence time and can be read out and initialized using nonresonant optical excitation, which has enabled a wide range of metrology and quantum information applications. At cryogenic temperatures, the NV center exhibits a variety of narrow, atom-like optical transitions, which has made the NV center a promising platform for quantum optics applications. We use coherent optical manipulation of the NV center at cryogenic temperatures to probe its internal dynamics and aspects of its interactions with its environment.\nFirst, we investigate the intersystem crossing (ISC) process, which is a spin-dependent nonradiative decay mechanism that enables the electronic spin state to be optically initialized and read out at room temperature. We measure the ISC rates from different excited states as well as the rate at which interactions with phonons redistribute population between these states. Based on these measurements, we develop a theoretical model that unifies the phonon-induced mixing and ISC mechanisms. We find that our model is in excellent agreement with experiment and that it can be used to predict unknown elements of the NV center's electronic structure.\nSecond, we investigate a novel method of using coherent optical manipulation of the NV center's electronic spin to control a nearby nuclear spin. Coherent interactions between the NV center and nearby nuclear spins have enabled the development of NV center-based, multi-qubit quantum registers, but these techniques have generally required the application of microwave or radio-frequency radiation. We demonstrate control of the nuclear spin using an all-optical Raman technique and theoretically evaluate the extent to which the intrinsic physics of the NV center limits the coherence of this Raman-based manipulation technique.
The nitrogen-vacancy (NV) center in diamond is of high importance in quantum information processing applications. The operation of the NV center relies on the efficient optical polarization of its electron spin. However, the full optical spin-polarization process, which involves the intersystem crossing between the shelving singlet state and the ground-state triplet, is not understood. Here we develop a detailed theory of this process which involves a combination of pseudo- and dynamic Jahn-Teller interactions together with spin-orbit interaction. Our theory provides an explanation for the asymmetry between the observed emission and absorption spectra of the singlet states. We apply density functional theory to calculate the intersystem crossing rates and the optical spectra of the singlets, and we obtain a good agreement with the experimental data. Since the NV center serves as a template for other solid-state-defect quantum bit systems, our theory provides a toolkit to study them that might help optimize their quantum bit operation.
Optical initialization of the negatively charged nitrogen-vacancy (NV${}^{\ensuremath{-}}$) center in diamond makes it one of the best candidates for realization of addressable spins in the solid state for quantum computing and other studies. However, its exact mechanism was not clear. We show that exact diagonalization of a many-electron Hamiltonian with parameters derived from ab initio GW calculations puts strong constraints on the mechanism. The energy surfaces of the low-energy many-body states and the relaxation processes of photoexcitation responsible for the optical initialization are calculated. Intersystem crossings are shown to be essential.