First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation
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.
Authors
- D. D. Awschalom (ORCID: https://orcid.org/0000-0002-8591-2687)
- Benchen Huang (ORCID: https://orcid.org/0000-0003-2003-725X)
- Marco Govoni (ORCID: https://orcid.org/0000-0001-6303-2403)
- F. Joseph Heremans (ORCID: https://orcid.org/0000-0003-3337-7958)
- Giulia Galli (ORCID: https://orcid.org/0000-0002-8001-5290)
- Benjamin Pingault (ORCID: https://orcid.org/0000-0003-1259-2747)
- Malcolm McMillan
- Christopher Egerstrom (ORCID: https://orcid.org/0000-0001-8240-7303)
- Jinsoo Park (ORCID: https://orcid.org/0000-0002-1763-5788)
- C. Barnes (ORCID: https://orcid.org/0000-0002-8750-5583)
- Daniel Donghyon Ohm
- Karl J. Friston
Institutions
- University of Modena and Reggio Emilia (IT)
- Argonne National Laboratory (US)
- Seoul National University (KR)
- University of Chicago (US)
Publication Details
- Journal
- Physical Review Letters
- Published
- 2025-06-16
- DOI
- https://doi.org/10.1103/nw3r-zy8q
- Citations
- 6
- Primary Topic
- Semiconductor materials and devices
- Type
- article
- Field-Weighted Citation Impact
- 4.38
Funders
- U.S. Department of Energy
- University of Chicago
- National Energy Research Scientific Computing Center
- Midwest Integrated Center for Computational Materials
- National Research Foundation of Korea
- Ministry of Science and ICT, South Korea
- Office of Science
- Multidisciplinary University Research Initiative
- Basic Energy Sciences
- Air Force Office of Scientific Research