First-principles theory of the luminescence lineshape for the triplet transition in diamond NV centres

Abstract

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 firstprinciples 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.

Multimode Jahn-Teller effect in bulk systems: A case of the NV0 center in diamond

“…The impact of the Jahn-Teller effect on the properties of the NV centers has been under investigation from the 1970s to the 1980s [13][14][15]. Recently, the vibronic properties and the JT effect of the NV − center have been continuously investigated by new experiments [11,16,17] and ab initio calculations [9,10,18,19]. The studies confirm the presence of the dynamic JT effect in the excited state of the NV − center [10,11].…”

“…We adopt the method introduced by Alkauskas et al to calculate the luminescence line shape and the Huang-Rhys (HR) factor for the neutral NV center [19]. The method has been used successfully in the study of the negatively charged NV center.…”

“…[19]. Taking the atomic positions of the energy minimum point M in the APES as a reference, the position deviation of point X from the energy minimum point M in the APES can be described by 3N equations:…”

Defect states in hexagonal boron nitride: Assignments of observed properties and prediction of properties relevant to quantum computation

“…These optimized supercells were then embedded in 10x10x1 supercells using a similar method as described in Ref. [38] for minimizing the computational cost for large calculations and to ensure no interaction in planer directions for the calculation of hyperfine coupling(HF) constants. An increased planewave cut-off of 500 eV was used, which was sufficient to obtain a converged spin density and HF coupling constants (A xx , A yy , A zz ), where A xx , A yy , A zz are the principle values of HF coupling tensor.…”

Scalable fabrication of coupled NV center - photonic crystal cavity systems by self-aligned N ion implantation

“…Furthermore, one has to differentiate between the overall Purcell enhancement F and the spectrally-resolved SE rate enhancement F ZPL = F/DW, with DW the Debye-Waller factor, i.e. the intensity ratio of the ZPL to the overall fluorescence [39]. When the NV ZPL is coupled to a cavity with quality factor Q and mode volume V mode , the enhancement is given by…”