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

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.Comment: 22 pages, 12 figure

Properties of donor qubits in ZnO formed by indium ion implantation

Shallow neutral donors (D$^\mathrm{0}$) in ZnO have emerged as a promising candidate for solid-state spin qubits. Here, we report on the formation of D$^\mathrm{0}$ in ZnO via implantation of In and subsequent annealing. The implanted In donors exhibit optical and spin properties on par with $\textit{in situ}$ doped donors. The inhomogeneous linewidth of the donor-bound exciton transition is less than 10 GHz, comparable to the optical linewidth of $\textit{in situ}$ In. Longitudinal spin relaxation times ($T_1$) exceed reported values for $\textit{in situ}$ Ga donors, indicating that residual In implantation damage does not degrade $T_1$. Two laser Raman spectroscopy on the donor spin reveals the hyperfine interaction of the donor electron with the spin-9/2 In nuclei. This work is an important step toward the deterministic formation of In donor qubits in ZnO with optical access to a long-lived nuclear spin memory

Ensemble spin relaxation of shallow donor qubits in ZnO

We present an experimental and theoretical study of the longitudinal electron spin relaxation ($T_1$) of shallow donors in the direct band-gap semiconductor ZnO. $T_1$ is measured via resonant excitation of the Ga donor-bound exciton. $T_1$ exhibits an inverse-power dependence on magnetic field $T_1\propto B^{-n}$, with $4\leq n\leq 5$, over a field range of 1.75 T to 7 T. We derive an analytic expression for the donor spin-relaxation rate due to spin-orbit (admixture mechanism) and electron-phonon (piezoelectric) coupling for the wurtzite crystal symmetry. Excellent quantitative agreement is found between experiment and theory suggesting the admixture spin-orbit mechanism is the dominant contribution to $T_1$ in the measured magnetic field range. Temperature and excitation-energy dependent measurements indicate a donor density dependent interaction may contribute to small deviations between experiment and theory. The longest $T_1$ measured is 480 ms at 1.75 T with increasing $T_1$ at smaller fields theoretically expected. This work highlights the extremely long longitudinal spin-relaxation time for ZnO donors due to their small spin-orbit coupling.Comment: 9 pages, 11 figure

Isolation of Single Donors in ZnO

The shallow donor in zinc oxide (ZnO) is a promising semiconductor spin qubit with optical access. Single indium donors are isolated in a commercial ZnO substrate using plasma focused ion beam (PFIB) milling. Quantum emitters are identified optically by spatial and frequency filtering. The indium donor assignment is based on the optical bound exciton transition energy and magnetic dependence. The single donor emission is intensity and frequency stable with a transition linewidth less than twice the lifetime limit. The isolation of optically stable single donors post-FIB fabrication is promising for optical device integration required for scalable quantum technologies based on single donors in direct band gap semiconductors.Comment: E. R. Hansen and V. Niaouris contributed equally to this work. 13 pages, 11 figure

Supplementary document for Contributions to the optical linewidth of shallow donor-bound excitonic transition in ZnO - 6740907.pdf

Supplament