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arXiv · 2502.19658

First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation

Yu Jin·Jinsoo Park·Marquis M. McMillan·Daniel Donghyon Ohm·Corrie Barnes·Benjamin Pingault·Christopher Egerstrom·Benchen Huang·Marco Govoni·F. Joseph Heremans·David D. Awschalom·Giulia Galli
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Abstract

Optically active spin defects in solids are promising platforms for quantum technologies. Here, we present a first-principles framework to investigate intersystem crossing processes, which represent crucial steps in the optical spin-polarization cycle used to address spin defects. Considering the nitrogen-vacancy center in diamond as a case study, we demonstrate that our framework effectively captures electron correlation effects in the calculation of many-body electronic states and their spin-orbit coupling and electron-phonon interactions, while systematically addressing finite-size effects. We validate our predictions by carrying out measurements of fluorescence lifetimes, finding excellent agreement between theory and experiments. The framework presented here provides a versatile and robust tool for exploring the optical cycle of varied spin defects entirely from first principles.

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Yu Jin, Jinsoo Park, Marquis M. McMillan, Daniel Donghyon Ohm, Corrie Barnes, Benjamin Pingault, Christopher Egerstrom, Benchen Huang, Marco Govoni, F. Joseph Heremans, David D. Awschalom, Giulia Galli. 2025-02-27. First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation. https://doi.org/10.1103/nw3r-zy8q

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