Contributions to the optical linewidth of shallow donor-bound excitonic transition in ZnO

Abstract

We study the donor-bound exciton optical linewidth properties of Al, Ga and In donor ensembles in single-crystal zinc oxide (ZnO). Neutral shallow donors (D$^0$) in ZnO are spin qubits with optical access via the donor-bound exciton (D$^0$X). This spin-photon interface enables applications in quantum networking, memories and transduction. Essential optical parameters which impact the spin-photon interface include radiative lifetime, optical inhomogeneous and homogeneous linewidth and optical depth. The ensemble photoluminescence linewidth ranges from 4-11 GHz, less than two orders of magnitude larger than the expected lifetime-limited linewidth. The ensemble linewidth remains narrow in absorption measurements through the 300 $\mu$m-thick sample, which has an estimated optical depth up to several hundred. Homogeneous broadening of the ensemble line due to phonons is consistent with thermal population relaxation between D$^0$X states. This thermal relaxation mechanism has negligible contribution to the total linewidth at 2 K. We find that inhomogeneous broadening due to the disordered isotopic environment in natural ZnO is significant, ranging from 1.9 GHz - 2.2 GHz. Two-laser spectral anti-hole burning measurements, which can be used to measure the homogeneous linewidth in an ensemble, however, reveal spectral anti-hole linewidths similar to the single laser ensemble linewidth. Despite this broadening, the high homogeneity, large optical depth and potential for isotope purification indicate that the optical properties of the ZnO donor-bound exciton are promising for a wide range of quantum technologies and motivate a need to improve the isotope and chemical purity of ZnO for quantum technologies.