Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

arXiv:2606.19016

Coherent Microwave Control of Optically Addressable Donor Qubits in ZnO

Ethan R. Hansen, Dong-Rong Wu, Yixuan Li, Yaser Silani, Joseph Falson, Yusuke Kozuka, Masashi Kawasaki, Yuan Ping, Kai-Mei C Fu

quant-phSubmitted Jun 17, 2026• Announced Jun 18, 2026
arXivHTMLPDF

Abstract

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 $^{115}\mathrm{In}$ 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 $^{115}\mathrm{In}$ nuclear spin (I = 9/2) and reveals optical-pumping-induced nuclear spin polarization. We observe coherent Rabi oscillations with a maximum Rabi frequency of $Ω/2π= 36.2 \pm 0.7$\;MHz, corresponding to a $π$-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.

Comments
14 pages, 15 figures

Related papers

Coherent Optical Control of a Single Donor Electron Spin

Yuxi Jiang, Amirehsan Alizadehherfati, Christine Falter +6 more

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.

quant-pharXiv:2610.36423•Oct 28, 2026

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

Xingyi Wang, Sai Mu, Jeong Rae Kim +6 more

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.

quant-pharXiv:2603.05615•Mar 9, 2026

Coherent electric field manipulation of nuclear spin qudit

Sumin Lim, Mikhail V. Vaganov, Niccolo Fontana +2 more

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.

quant-pharXiv:2607.26716•Jul 30, 2026

Quantum control of nuclear-spin qubits in a rapidly rotating diamond

A. A. Wood, R. M. Goldblatt, Robert E Scholten +1 more

Nuclear spins in certain solids couple weakly to their environment, making them attractive candidates for quantum information processing and inertial sensing. When coupled to the spin of an optically active electron, nuclear spins can be rapidly polarized, controlled, and read via lasers and radio-frequency (rf) fields. Possessing typical coherence times of several milliseconds at room temperature, nuclear spins hosted by a nitrogen-vacancy center in diamond are thus intriguing systems to observe how classical physical rotation at quantum timescales affects a quantum system. In this work, we demonstrate optical nuclear-spin polarization and rapid quantum control of nuclear spins in a diamond physically rotating at $1\phantom{\rule{0.16em}{0ex}}\mathrm{kHz}$, faster than the nuclear-spin coherence time. Free from the need to maintain strict field alignment, we are able to measure and control nuclear spins in the presence of a large, time-varying magnetic field that makes an angle of more than ${100}^{\ensuremath{\circ}}$ to the nitrogen-lattice vacancy axis. The field induces spin mixing between the electron and nuclear states of the qubits, decoupling them from oscillating rf fields. We are able to demonstrate that coherent spin state control is possible at any point of the rotation. We combine continuous dynamical decoupling with feed-forward control to eliminate decoherence induced by imperfect mechanical rotation. Our work liberates a previously inaccessible degree of freedom of the NV nuclear spin, unlocking new approaches to quantum control and rotation sensing.

arXiv:2107.12577•Physical Review Research•Dec 13, 2021•14 citations

Robust electric dipole transition at microwave frequencies for nuclear spin qubits in silicon

G. Tosi, Fahd A. Mohiyaddin, Stefanie Tenberg +2 more

The nuclear spin state of a phosphorus donor ($^{31}\mathrm{P}$) in isotopically enriched silicon-28 is an excellent host to store quantum information in the solid state. The spin's insensitivity to electric fields yields a solid-state qubit with record coherence times but also renders coupling to other quantum systems very challenging. Here, we describe how to generate a strong electric dipole ($>100$ D) at microwave frequencies for the nuclear spin. This is achieved by applying a magnetic drive to the spin of the donor-bound electron while simultaneously controlling its charge state with electric fields. Under certain conditions, the microwave magnetic drive also renders the nuclear spin resonance frequency and electric dipole strongly insensitive to electrical noise, yielding long ($>1$ ms) dephasing times and robust gate operations. The nuclear spin could then be strongly coupled to microwave resonators, with a vacuum Rabi splitting of the order of 1 MHz, or to other nuclear spins, nearly half a micrometer apart, via strong electric dipole-dipole interaction. This work brings the $^{31}\mathrm{P}$ nuclear qubit into the realm of hybrid quantum systems and opens up new avenues in quantum information processing.

arXiv:1706.08095•Physical review. B./Physical review. B•Aug 30, 2018•20 citations

Optical Detection of Coherent Nuclear Spin Control in a Molecular System at Room Temperature

Eoin O. Irving, Ziqiu Huang, Max Attwood +2 more

Molecular systems with optically addressable electron spins are emerging as versatile quantum sensing platforms, offering tunable qubit properties and molecular-scale spatial control. Owing to their longer lifetimes, coupled nuclear spins provide an attractive resource for enhancing sensing performance. For molecular spin systems, the ability to initialise, coherently control and readout nuclear spins at room temperature is crucial for realising such benefits. Here, we present the first optical detection of nuclear magnetic resonance and coherent nuclear spin control with a molecular system at room temperature. Specifically, we demonstrate optically detected Rabi oscillations of $^{14}$N nuclear spins in the photoexcited triplet state of the organic chromophore 6,13-diazapentacene. The strong hyperfine coupling between the electronic spin and $^{14}$N nuclei enhances the nuclear Rabi frequency, enabling fast coherent nuclear-spin rotations. This work lays the foundation for leveraging nuclear spins as memories for enhanced molecular-based quantum sensing.

quant-pharXiv:2610.17050•Oct 13, 2026
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.
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.
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.
Nuclear spins in certain solids couple weakly to their environment, making them attractive candidates for quantum information processing and inertial sensing. When coupled to the spin of an optically active electron, nuclear spins can be rapidly polarized, controlled, and read via lasers and radio-frequency (rf) fields. Possessing typical coherence times of several milliseconds at room temperature, nuclear spins hosted by a nitrogen-vacancy center in diamond are thus intriguing systems to observe how classical physical rotation at quantum timescales affects a quantum system. In this work, we demonstrate optical nuclear-spin polarization and rapid quantum control of nuclear spins in a diamond physically rotating at 1kHz1\phantom{\rule{0.16em}{0ex}}\mathrm{kHz}1kHz, faster than the nuclear-spin coherence time. Free from the need to maintain strict field alignment, we are able to measure and control nuclear spins in the presence of a large, time-varying magnetic field that makes an angle of more than ${100}^{\ensuremath{\circ}}$ to the nitrogen-lattice vacancy axis. The field induces spin mixing between the electron and nuclear states of the qubits, decoupling them from oscillating rf fields. We are able to demonstrate that coherent spin state control is possible at any point of the rotation. We combine continuous dynamical decoupling with feed-forward control to eliminate decoherence induced by imperfect mechanical rotation. Our work liberates a previously inaccessible degree of freedom of the NV nuclear spin, unlocking new approaches to quantum control and rotation sensing.
The nuclear spin state of a phosphorus donor (31P^{31}\mathrm{P}31P) in isotopically enriched silicon-28 is an excellent host to store quantum information in the solid state. The spin's insensitivity to electric fields yields a solid-state qubit with record coherence times but also renders coupling to other quantum systems very challenging. Here, we describe how to generate a strong electric dipole (>100>100>100 D) at microwave frequencies for the nuclear spin. This is achieved by applying a magnetic drive to the spin of the donor-bound electron while simultaneously controlling its charge state with electric fields. Under certain conditions, the microwave magnetic drive also renders the nuclear spin resonance frequency and electric dipole strongly insensitive to electrical noise, yielding long (>1>1>1 ms) dephasing times and robust gate operations. The nuclear spin could then be strongly coupled to microwave resonators, with a vacuum Rabi splitting of the order of 1 MHz, or to other nuclear spins, nearly half a micrometer apart, via strong electric dipole-dipole interaction. This work brings the 31P^{31}\mathrm{P}31P nuclear qubit into the realm of hybrid quantum systems and opens up new avenues in quantum information processing.
Molecular systems with optically addressable electron spins are emerging as versatile quantum sensing platforms, offering tunable qubit properties and molecular-scale spatial control. Owing to their longer lifetimes, coupled nuclear spins provide an attractive resource for enhancing sensing performance. For molecular spin systems, the ability to initialise, coherently control and readout nuclear spins at room temperature is crucial for realising such benefits. Here, we present the first optical detection of nuclear magnetic resonance and coherent nuclear spin control with a molecular system at room temperature. Specifically, we demonstrate optically detected Rabi oscillations of 14^{14}14N nuclear spins in the photoexcited triplet state of the organic chromophore 6,13-diazapentacene. The strong hyperfine coupling between the electronic spin and 14^{14}14N nuclei enhances the nuclear Rabi frequency, enabling fast coherent nuclear-spin rotations. This work lays the foundation for leveraging nuclear spins as memories for enhanced molecular-based quantum sensing.