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arXiv:0910.0494 · Physical Review Letters

Observation of the Dynamic Jahn-Teller Effect in the Excited States of Nitrogen-Vacancy Centers in Diamond

Kai‐Mei C. Fu, Charles Santori, Paul E. Barclay, Lachlan J. Rogers, Neil B. Manson, Raymond G. Beausoleil

Published Dec 17, 2009• 265 citations
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Abstract

The optical transition linewidth and emission polarization of single nitrogen-vacancy (NV) centers are measured from 5 K to room temperature. Interexcited state population relaxation is shown to broaden the zero-phonon line and both the relaxation and linewidth are found to follow a T(5) dependence for T < 100 K. This dependence indicates that the dynamic Jahn-Teller effect is the dominant dephasing mechanism for the NV optical transitions at low temperatures.

DOI
10.1103/physrevlett.103.256404

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The optical transition linewidth and emission polarization of single nitrogen-vacancy (NV) centers are measured from 5 K to room temperature. Interexcited state population relaxation is shown to broaden the zero-phonon line and both the relaxation and linewidth are found to follow a T(5) dependence for T < 100 K. This dependence indicates that the dynamic Jahn-Teller effect is the dominant dephasing mechanism for the NV optical transitions at low temperatures.
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.
The negatively charged nitrogen-vacancy (NV(-)) center in diamond is considered to be one of the most promising solid state systems for quantum information applications. Excited states of the NV(-) center play a center role in the proposed applications. Using a combination of first-principles calculations and vibronic interaction model analysis, we establish the presence of a dynamic Jahn-Teller effect in the (3)E excited state. The calculated temperature-dependent dephasing rate for the zero phonon line as well as the splitting of the first two vibronic states are in good agreement with experiment.
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.
Abstract Many applications of nitrogen-vacancy (NV) centers in diamond crucially rely on a spectrally narrow and stable optical zero-phonon line transition. Though many impressive proof-of-principle experiments have been demonstrated, much work remains in engineering NV centers with spectral properties that are sufficiently robust for practical implementation. To elucidate the mechanisms underlying their interactions with the environment, we apply multi-dimensional coherent spectroscopy to an NV center ensemble in bulk diamond at cryogenic temperatures. Our spectra reveal thermal dephasing due to quasi-localized vibrational modes as well as ultrafast spectral diffusion on the picosecond timescale. The intrinsic, ensemble-averaged homogeneous linewidth is found to be in the tens of GHz range by extrapolating to zero temperature. We also observe a temperature-dependent Stark splitting of the excited state manifold, relevant to NV sensing protocols.
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