A first-principles calculation of electron-phonon interactions for the $\text{C}_2\text{C}_\text{N}$ and $\text{V}_\text{N}\text{N}_\text{B}$ defects in hexagonal boron nitride

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. The mechanism responsible for the narrow lines has been suggested to be a mechanical decoupling from in-plane phonons due to an out-of-plane distortion of the emitter's orbitals. All decoupled emitters produce photons that are directed in-plane, suggesting that the dipoles are oriented 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 $\text{C}_2 \text{C}_\text{N}$ defect has an in-plane transition dipole moment, and that of the $\text{V}_\text{N} \text{N}_\text{B}$ defect is perpendicular to the plane. We exploit the two-dimensional framework recently implemented in \texttt{QUANTUM ESPRESSO} to determine 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 is sufficient to obtain FT-limited photons at room temperature. Our work also 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.