State-selective intersystem crossing in nitrogen-vacancy centers

TL;DR

This paper presents a microscopic model of the state-selective intersystem crossing in nitrogen-vacancy centers in diamond, linking electron-phonon interactions to population dynamics and optical properties, consistent with recent measurements.

Contribution

It introduces a detailed microscopic model of ISC in NV centers that correlates electron-phonon interactions with population dynamics and optical features, providing new insights into energy level spacings.

Findings

Model aligns with recent ISC measurements

Constrains energy spacings between spin states

Suggests engineering approaches to improve spin readout

Abstract

The intersystem crossing (ISC) is an important process in many solid-state atomlike impurities. For example, it allows the electronic spin state of the nitrogen-vacancy (NV) center in diamond to be initialized and read out using optical fields at ambient temperatures. This capability has enabled a wide array of applications in metrology and quantum information science. Here, we develop a microscopic model of the state-selective ISC from the optical excited state manifold of the NV center. By correlating the electron-phonon interactions that mediate the ISC with those that induce population dynamics within the NV center's excited state manifold and those that produce the phonon sidebands of its optical transitions, we quantitatively demonstrate that our model is consistent with recent ISC measurements. Furthermore, our model constrains the unknown energy spacings between the center's spin-singlet and spin-triplet levels. Finally, we discuss prospects to engineer the ISC in order to improve the spin initialization and readout fidelities of NV centers.