Accurate and convergent energetics of color centers by wavefunction theory
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Tartalom: https://real.mtak.hu/247842/
Archívum: REAL
Gyűjtemény: Status = Published
Subject = Q Science / természettudomány: QC Physics / fizika: QC06 Physics of condensed matter / szilárdtestfizika
Type = Article
Cím:
Accurate and convergent energetics of color centers by wavefunction theory
Létrehozó:
Benedek, Zsolt
Ganyecz, Ádám
Pershin, Anton
Ivády, Viktor
Barcza, Gergely
Dátum:
2025
Téma:
QC06 Physics of condensed matter / szilárdtestfizika
Tartalmi leírás:
The accurate description of in-gap states of point defects in semiconductors with significant multideterminant character presents a long-standing challenge for density functional theory (DFT) methods. In this study, we devise an ab initio methodology based on wavefunction theory (WFT) as a competing alternative approach. Specifically, we apply perturbation theory (NEVPT2) on top of a defect-localized many-body wavefunction (CASSCF). This quantum chemistry methodology, exemplified for the NV− center in diamond, is not only used for the calculation of energies and properties, but also for state-specific geometry optimization. By relaxing cluster models of increasing size and investigating convergence behavior, we accurately computed (i) the energy levels of NV− electronic states involved in the polarization cycle, (ii) the effect of Jahn-Teller distortion on measurable properties, (iii) the fine structure of ground and excited states, and (iv) the pressure dependence of zero-phonon lines. In addition, we predict hitherto uncharacterized high-lying excited states.
Nyelv:
angol
Típus:
Article
PeerReviewed
Formátum:
text
Azonosító:
Benedek, Zsolt and Ganyecz, Ádám and Pershin, Anton and Ivády, Viktor and Barcza, Gergely (2025) Accurate and convergent energetics of color centers by wavefunction theory. npj Computational Materials, 11 (1). No.-346. ISSN 2057-3960
Kapcsolat:
doi:10.1038/s41524-025-01813-0
Létrehozó:
cc_by_nc_nd