Phonon-Induced Population Dynamics and Intersystem Crossing in Nitrogen-Vacancy Centers

TL;DR

This study measures and models the population dynamics, phonon-induced mixing, and intersystem crossing in nitrogen-vacancy centers in diamond, providing insights for improving their use in room-temperature sensing.

Contribution

It introduces a comprehensive theoretical model that unifies phonon-induced mixing and intersystem crossing mechanisms in NV centers, validated by experimental data.

Findings

Phonon-induced mixing rate can be suppressed at low temperatures.

The developed model accurately predicts the electronic structure elements.

Insights for enhancing NV center performance as sensors.

Abstract

We report direct measurement of population dynamics in the excited state manifold of a nitrogen-vacancy (NV) center in diamond. We quantify the phonon-induced mixing rate and demonstrate that it can be completely suppressed at low temperatures. Further, we measure the intersystem crossing (ISC) rate for different excited states and 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. We discuss the model's implications for enhancing the NV center's performance as a room-temperature sensor.