2014/05/28 by Audrius Alkauskas, Bob B. Buckley, David D. Awschalom +2 · 5 citations
Earth and Planetary Sciences · Materials Science · Physics and Astronomy · #Atomic physics #Condensed matter physics #Coupling (piping) #Diamond #Diamond and Carbon-based Materials Research #Electron #Electronic and Structural Properties of Oxides #High-pressure geophysics and materials #Luminescence #Materials science #Optoelectronics #Phonon #Physics #Quantum mechanics #Vacancy defect #cond-mat.mes-hall
paper · pdf · doi:10.1088/1367-2630/16/7/073026
published as New J. Phys. 16, 073026 (2014)
arxiv created 2014/05/28 · openalex publication_date 2014/07/17 · arxiv updated 2015/03/25 · openalex created_date 2016/06/24 · openalex updated_date 2026/08/06
In this work we present theoretical calculations and analysis of the vibronic structure of the spin-triplet optical transition in diamond nitrogen-vacancy (NV) centres. The electronic structure of the defect is described using accurate first-principles methods based on hybrid functionals. We devise a computational methodology to determine the coupling between electrons and phonons during an optical transition in the dilute limit. As a result, our approach yields a smooth spectral function of electron–phonon coupling and includes both quasi-localized and bulk phonons on equal footings. The luminescence lineshape is determined via the generating function approach. We obtain a highly accurate description of the luminescence band, including all key parameters such as the Huang–Rhys factor, the Debye–Waller factor, and the frequency of the dominant phonon mode. More importantly, our work provides insight into the vibrational structure of NV centres, in particular the role of local modes and vibrational resonances. In particular, we find that the pronounced mode at 65 meV is a vibrational resonance, and we quantify localization properties of this mode. These excellent results for the benchmark diamond (NV) centre provide confidence that the procedure can be applied to other defects, including alternative systems that are being considered for applications in quantum information processing.