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arXiv:2603.05615

Identification of the I$_{10}$ Donor in ZnO as a Sn--Li Complex with Large Hyperfine Interaction

Xingyi Wang, Sai Mu, Jeong Rae Kim, Ethan R. Hansen, Yaser Silani, Lasse Vines, Joseph Falson, Chris G. Van de Walle, Kai-Mei C. Fu

quant-phSubmitted Mar 5, 2026• Announced Mar 9, 2026
arXivHTMLPDF

Abstract

Donor impurities in wide direct band gap semiconductors provide a promising platform for spin--photon quantum technologies by combining a donor spin qubit with optically addressable transitions. In ZnO, the shallow donor with the largest reported binding energy has long been associated with the I$_{10}$ bound exciton line, but its microscopic origin has remained unresolved. Here we demonstrate the controlled formation and identification of this donor as a Sn--Li complex through a combination of ion implantation, annealing, optical spectroscopy, and first-principles calculations. Resonant two-laser coherent population trapping measurements reveal an electron--$^{119}$Sn hyperfine interaction of $392 \pm 15$\,MHz, establishing a coupled electron--spin--1/2, nuclear--spin--1/2 system with one of the largest hyperfine couplings reported for shallow donors in semiconductors. Density functional theory calculations show that a nearest-neighbor Sn$_{\mathrm{Zn}}$--Li$_{\mathrm{Zn}}$ complex has favorable formation energetics, donor character with the electron localized on Sn, and an extrapolated hyperfine interaction consistent with experiment. The large donor binding energy and excited-state structure indicate enhanced thermal robustness of the optical transition relative to conventional group--III donors, while the strong hyperfine interaction enables fast electron--nuclear spin control and prospects for direct nuclear--spin--photon interfaces. We further observe efficient optically induced nuclear spin polarization, highlighting a path toward nuclear spin initialization. More broadly, our results reveal how a donor--acceptor complex can access previously unexplored regimes of shallow donor physics, extending the design space of quantum defects beyond isolated substitutional dopants.

Comments
10 pages, 7 figures

Related papers

Coherent Microwave Control of Optically Addressable Donor Qubits in ZnO

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•Jan 1, 2015•1 citation

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Spins in condensed matter, especially well-isolated nuclear spins, offer attractive quantum degrees of freedom for computing, sensing, and networking because of their long coherence times. The possibility of electric-field control is an important feature for practical scalable quantum technologies, but, typically, nuclear spins couple only weakly to electric fields in conventional semiconductor hosts, limiting operation efficiency. Here we show that a choice of a highly polarizable oxide host can overcome this bottleneck. In Mn2+ doped ZnO, electric-field modulation of the spin Hamiltonian is amplified by hyperfine-coupled electron spins, and offers efficient electric-field manipulation of an I = 5/2 nuclear spin qudit, in a manner analogous to the hyperfine enhancement of conventional nuclear magnetic resonance. We demonstrate both resonant and non-resonant coherent manipulation using a single uniaxial electric field applied along the crystalline c-axis, the polarization axis of ZnO. This approach allows universal single-qudit gate operations with efficiencies comparable to or exceeding those of conventional magnetic-field driving. These results support the deployment of doped oxides as active host materials for electrically controllable spin qubits, highlighting the importance of materials design in developing scalable quantum technologies.

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Identification of the I10_{10}10​ Donor in ZnO as a Sn--Li Complex with Large Hyperfine Interaction
Donor impurities in wide direct band gap semiconductors provide a promising platform for spin--photon quantum technologies by combining a donor spin qubit with optically addressable transitions. In ZnO, the shallow donor with the largest reported binding energy has long been associated with the I10_{10}10​ bound exciton line, but its microscopic origin has remained unresolved. Here we demonstrate the controlled formation and identification of this donor as a Sn--Li complex through a combination of ion implantation, annealing, optical spectroscopy, and first-principles calculations. Resonant two-laser coherent population trapping measurements reveal an electron--119^{119}119Sn hyperfine interaction of 392±15392 \pm 15392±15,MHz, establishing a coupled electron--spin--1/2, nuclear--spin--1/2 system with one of the largest hyperfine couplings reported for shallow donors in semiconductors. Density functional theory calculations show that a nearest-neighbor SnZn_{\mathrm{Zn}}Zn​--LiZn_{\mathrm{Zn}}Zn​ complex has favorable formation energetics, donor character with the electron localized on Sn, and an extrapolated hyperfine interaction consistent with experiment. The large donor binding energy and excited-state structure indicate enhanced thermal robustness of the optical transition relative to conventional group--III donors, while the strong hyperfine interaction enables fast electron--nuclear spin control and prospects for direct nuclear--spin--photon interfaces. We further observe efficient optically induced nuclear spin polarization, highlighting a path toward nuclear spin initialization. More broadly, our results reveal how a donor--acceptor complex can access previously unexplored regimes of shallow donor physics, extending the design space of quantum defects beyond isolated substitutional dopants.
Optically addressable shallow donors in ZnO combine efficient spin-selective optical transitions with the potential for long spin coherence in an isotopically purifiable host lattice, making them an attractive platform for spin-photon quantum technologies. A key missing capability, however, has been coherent control beyond the small-angle rotations accessible with ultrafast optical pulses. Here we demonstrate coherent microwave control of implanted 115In^{115}\mathrm{In}115In donors in ZnO. Resonant optical pumping initializes and reads out the donor electron spin. Pulsed optically-detected magnetic resonance resolves the ten hyperfine transitions associated with the coupled 115In^{115}\mathrm{In}115In nuclear spin (I = 9/2) and reveals optical-pumping-induced nuclear spin polarization. We observe coherent Rabi oscillations with a maximum Rabi frequency of Ω/2π=36.2±0.7Ω/2π= 36.2 \pm 0.7Ω/2π=36.2±0.7\;MHz, corresponding to a πππ-pulse time of 13.8$\pm$0.3\;ns, and characterize the spin coherence using Ramsey, Hahn echo and dynamical-decoupling measurements. Unexpectedly, the measured coherence is substantially shorter than reported in previous optical studies of donor spins in ZnO at high magnetic field. Control experiments rule out several simple explanations including microwave heating and instantaneous diffusion from the driven donor ensemble, leaving an open question regarding the origin of decoherence at low magnetic field in microwave-controlled ZnO donors. These results establish microwave control of ZnO donor qubits with resonant optical access to specific donor species. More broadly, they demonstrate that coherent microwave control can be achieved in optically addressable spin systems with nanosecond-scale inhomogeneous dephasing, enabling field-, temperature-, and materials-dependent studies of coherence-limiting mechanisms and the development of optically interfaced electron-nuclear spin registers.
Coherent spin-photon interfaces are essential for scalable quantum networks, but their realization requires optically bright transitions, long-lived spin coherence, and complete coherent control. Donor-bound electron spins in II-VI semiconductors offer an attractive platform for optically active spin qubits because they combine strong donor-bound exciton transitions in a direct-bandgap material with a potentially nuclear-spin-free environment. However, coherent control of an individual optically active donor spin has remained elusive. Here we demonstrate optical initialization, coherent control, and readout of a single donor-bound electron spin in ZnSe. Using spin-selective donor-bound exciton optical transitions, we initialize the electron spin and directly resolve its spin-relaxation dynamics. We achieve coherent spin control with off-resonant picosecond optical pulses, as demonstrated by spin Rabi oscillations and Ramsey interference. We further coherently drive two spin-selective optical transitions and observe high-contrast coherent population trapping, demonstrating the formation of an optically controlled dark state. At higher driving strengths, multiple dark resonances reveal the hyperfine interaction between the electron and the I = 3/2 Cl nucleus. These results establish the first coherent optical control of a single donor electron spin in a II-VI semiconductor and identify isolated optical donors as a promising platform for solid-state optically active qubits.
Zinc oxide (ZnO), a wide-band-gap semiconductor with mature growth techniques, is a promising host for optically active quantum spins. Yet, optically active quantum defects in ZnO remain largely unexplored. Here, we identify and characterize a family of double substitutional impurities in ZnO, formed by main-group donor-acceptor (DA) pairs, as candidates for optically active quantum defects. Using hybrid density functional theory (DFT), we systematically investigate double substitutional DA complexes and their defect physics, including electronic structure, thermodynamic stability, and optical properties. The proposed defects exhibit isolated defect states, strong spin localization on the acceptor site, and C3vC_{3v}C3v​ symmetry. Importantly, the electronic structure of the DA pairs is largely determined by the atomic properties of their constituent atoms. We further examine their optical characteristics, including zero-phonon lines (ZPLs), radiative lifetimes, and nonradiative decay to assess their viability as color centers. Notably, among the dimers, (SiZn_{Zn}Zn​-BO_OO​)+^++ and (GeZn_{Zn}Zn​-BO_OO​)+^++ exhibit visible optical transitions with sub-microsecond radiative lifetimes and robust charge states against optical ionization, while (SiZn_{Zn}Zn​-CO_OO​)2+^{2+}2+ shows the smallest Huang-Rhys factor, approximately 5.6. Our results propose a new family of main-group donor-acceptor defects in ZnO as promising candidates for optically active spin defects.
Semiconductor hole spins offer a pathway to extended coherence times by decoupling from nuclear magnetic noise, while their spin-orbit coupling enables fast all-electrical control. In ZnSe, however, realizing this potential has been limited by p-doping challenges. Here, we circumvent this limit by optically activating acceptors within the ZnSe quantum well. We isolate a single-hole spin bound to a shallow acceptor, confirmed by antibunching and accessed via the fast (244 ps) radiative recombination of a bound exciton. Magnetic and Raman spectroscopy of the ground state reveal an effective hole g-factor of 0.7 and an optical resonance linewidth of 26.7 GHz. Complementary first-principles simulations, together with the experimental results, provide evidence that points toward nitrogen as the most likely acceptor impurity. These results introduce a promising new platform for optically active spin qubits and single-photon sources in ZnSe.
Donors in silicon, which combine an electron and nuclear spin, are some of the most promising candidates for quantum information. The electron spin has been proposed as a register with fast manipulation and the nuclear spin as a memory with long coherence times. However, this division reduces the complexity of the donor system, in particular behaviors emerging from their interaction. In natural silicon, there is also the presence of 29Si nuclear spins in the donor environment; though they are generally seen as a source of decoherence, they are quantum systems that can be investigated too. The main subject of this thesis is the study of the interactions between these various spins, using different methods to probe and control them. I first concentrate on the coupling between the donor and the 29Si spins. This coupling can be perturbed by the application of dynamical decoupling on the donor electron spin, whose evolution can be made sensitive to the number of 29Si spins interacting together. I then propose an error correction scheme using the donor and 29Si spins, showing key requirements such as coherence times and methods for manipulation and initialization. Secondly, I focus on the donor itself, in a regime where the hyperfine and Zeeman couplings compete with each other. Here, the spin transitions can have different sensitivities to the magnetic environment, and can even be suppressed to first order, resulting in coherence times up to seconds with electron spin-like manipulation times. Controlling this sensitivity was also used to probe the effect of the donor on the 29Si spin bath evolution. Finally, I use electric fields to modulate the hyperfine coupling within the donor. I first characterize the spins’ sensitivity to the electric field, and then demonstrate electrical switching of the nuclear spin response to an external magnetic excitation.
Spins in condensed matter, especially well-isolated nuclear spins, offer attractive quantum degrees of freedom for computing, sensing, and networking because of their long coherence times. The possibility of electric-field control is an important feature for practical scalable quantum technologies, but, typically, nuclear spins couple only weakly to electric fields in conventional semiconductor hosts, limiting operation efficiency. Here we show that a choice of a highly polarizable oxide host can overcome this bottleneck. In Mn2+ doped ZnO, electric-field modulation of the spin Hamiltonian is amplified by hyperfine-coupled electron spins, and offers efficient electric-field manipulation of an I = 5/2 nuclear spin qudit, in a manner analogous to the hyperfine enhancement of conventional nuclear magnetic resonance. We demonstrate both resonant and non-resonant coherent manipulation using a single uniaxial electric field applied along the crystalline c-axis, the polarization axis of ZnO. This approach allows universal single-qudit gate operations with efficiencies comparable to or exceeding those of conventional magnetic-field driving. These results support the deployment of doped oxides as active host materials for electrically controllable spin qubits, highlighting the importance of materials design in developing scalable quantum technologies.