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

TL;DR

This study provides a detailed first-principles analysis of the multimode Jahn-Teller effect in the excited state of the NV center in diamond, revealing mode-specific contributions and their implications for quantum technology applications.

Contribution

It offers the first microscopic, mode-resolved understanding of vibronic coupling in the NV center's excited state using density functional theory and distortion path analysis.

Findings

Multiple vibrational modes cooperatively participate in Jahn-Teller dynamics.

The potential energy surface is shallow with low barriers, enabling thermally activated pseudorotation.

Vibrational features align with two-dimensional electronic spectroscopy observations.

Abstract

We present a first-principles study of the multimode Jahn-Teller (JT) effect in the exctied $^{3}E$ 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.