First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation
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arXiv
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| Autori principali: | , , , , , , , , , , , |
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| Natura: | Preprint |
| Pubblicazione: |
2025
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| _version_ | 1866913949209853952 |
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| author | Jin, Yu Park, Jinsoo McMillan, Marquis M. Ohm, Daniel Donghyon Barnes, Corrie Pingault, Benjamin Egerstrom, Christopher Huang, Benchen Govoni, Marco Heremans, F. Joseph Awschalom, David D. Galli, Giulia |
| author_facet | Jin, Yu Park, Jinsoo McMillan, Marquis M. Ohm, Daniel Donghyon Barnes, Corrie Pingault, Benjamin Egerstrom, Christopher Huang, Benchen Govoni, Marco Heremans, F. Joseph Awschalom, David D. Galli, Giulia |
| contents | 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2502_19658 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation Jin, Yu Park, Jinsoo McMillan, Marquis M. Ohm, Daniel Donghyon Barnes, Corrie Pingault, Benjamin Egerstrom, Christopher Huang, Benchen Govoni, Marco Heremans, F. Joseph Awschalom, David D. Galli, Giulia Materials Science Quantum Physics 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. |
| title | First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation |
| topic | Materials Science Quantum Physics |
| url | https://arxiv.org/abs/2502.19658 |