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

• URL: http://arxiv.org/abs/2502.19658v1
• Date: Thu, 27 Feb 2025 01:01:24 GMT
• Title: First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation
• Authors: 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,
• Abstract summary: We present a first-principles framework to investigate intersystem crossing processes, which represent crucial steps in the optical spin-polarization cycle.<n>Considering the nitrogen-vacancy center in diamond as a case study, we demonstrate that our framework effectively captures electron correlation effects.<n>We validate our predictions by carrying out measurements of fluorescence lifetimes, finding excellent agreement between theory and experiments.
• Score: 1.9408226857225095
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• 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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