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Bulletin of the American Physical Society

Dynamic Jahn-Teller Effect in Negatively Charged Nitrogen-Vacancy Center in Diamond

Tesfaye A. Abtew, Peihong Zhang

Published Mar 23, 2011• 0 citations
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We present a first-principles study of the multimode Jahn-Teller (JT) effect in the exctied 3E^{3}E3E state of the negatively charged nitrogen-vacancy (NV) center in diamond. Using density functional theory combined with an intrinsic distortion path (IDP) analysis, we resolve the full activation pathways of the JT distortion and quantitatively decompose the distortion into contributions from individual vibrational modes. We find that multiple vibrational modes participate cooperatively in the JT dynamics, giving rise to a shallow adiabatic potential energy surface with low barriers, consistent with thermally activated pseudorotation. The dominant JT-active modes are found to closely correspond to vibrational features observed in two-dimensional electronic spectroscopy (2DES), in agreement with recent ab initio molecular dynamics simulations. Our results establish a microscopic, mode-resolved picture of vibronic coupling in the excited-state NV center and provide new insight into dephasing, relaxation, and optically driven dynamics relevant to solid-state quantum technologies.
The understanding of the coherence properties of photons emitted from negatively charged nitrogen-vacancy (NV) centers in diamond is essential for the success of quantum information applications based on indistinguishable photons. Here we study both the polarization of photons emitted from and the linewidth of photons absorbed by single NV centers as a function of temperature T. We find that for T < 100 K the main dephasing mechanism contributing to the linewidth broadening is phonon-mediated population transfer between the two excited orbital states. The observed T5 temperature dependence of the population transfer rate and linewidth is experimental evidence of a dynamic Jahn-Teller effect in the excited states.