A DFT study of electron–phonon interactions for the C2CN and VNNB defects in hexagonal boron nitride: investigating the role of the transition dipole direction

Abstract

Quantum emitters in two-dimensional hexagonal boron nitride (h-BN) have generated significant interest due to observations of ultra-bright emission made at room temperature. The expectation that solid-state emitters exhibit broad zero-phonon lines at elevated temperatures has been put in question by recent observations of Fourier transform (FT) limited photons emitted from h-BN flakes at room temperature. All decoupled emitters produce photons that are directed in-plane, suggesting that the dipoles are perpendicular to the h-BN plane. Motivated by the promise of an efficient and scalable source of indistinguishable photons that can operate at room temperature, we have developed an approach using density functional theory (DFT) to determine the electron- phonon coupling for defects that have in- and out-of-plane transition dipole moments. Our DFT calculations reveal that the transition dipole for the C2CN defect is parallel to the h-BN plane, and for the VNNB defect is perpendicular to the plane. We calculate both the phonon density of states and the electron-phonon matrix elements associated with the h-BN defective structures. We find no indication that an out-of-plane transition dipole by itself will result in the low electron-phonon coupling that is expected to produce FT-limited photons at room temperature. Our work provides direction to future DFT software developments and adds to the growing list of calculations relevant to researchers in the field of solid-state quantum information processing.

Solid‐State Single‐Photon Sources: Recent Advances for Novel Quantum Materials

“…A follow-up experiment gave evidence that an out-of-plane distortion can decouple the emitter from low-energy phonons, an effect that also persists up to room temperature. [251] However, recent density functional theory (DFT) simulations suggest that an out-of-plane distortion is not sufficient to provide hBN defects with Fourier-Transform limited lines at room temperature, [252] and so the exact decoupling phenomenon may be more complicated. Other experiments show substantial homogeneous broadening of hBN defect lines at room temperature, [85,86] indicating that Fourier Transform-limited lines are not a common feature of hBN defects.…”