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Semiconductor spin qubits have recently seen major advances in coherence time and control fidelities, leading to a single-qubit performance that is on par with other leading qubit platforms. Most of this progress is based on microwave control of single spins in devices made of isotopically purified silicon. For controlling spins, the exchange interaction is an additional key ingredient which poses new challenges for high-fidelity control. Here, we demonstrate exchange-based single-qubit gates of two-electron spin qubits in GaAs double quantum dots. Using careful pulse optimization and closed-loop tuning, we achieve a randomized benchmarking fidelity of (99.50±0.04)% and a leakage rate of 0.13% out of the computational subspace. These results open new perspectives for microwave-free control of singlet-triplet qubits in GaAs and other materials. The exchange interaction between spins poses considerable challenges for high-fidelity control of semiconductor spin qubits. Here, the authors use pulse optimization and closed-loop control to achieve a gate fidelity of 99.5% for exchange-based single-qubit gates of two-electron spin qubits in GaAs.

A controlled NOT gate for two quantum bits is demonstrated with a strained-silicon device Quantum computing could enable exponential speedups for certain classes of problems by exploiting superposition and entanglement in the manipulation of quantum bits (qubits). The leading quantum systems that can be used include trapped ions, superconducting qubits, and spins in semiconductors. The latter are considered particularly promising for scaling to very large numbers of qubits. On page 439 of this issue, Zajac et al. ( 1 ) demonstrate a quantum operation involving two qubits in silicon (Si), which is a major step for the field of semiconductor qubits. Together with easier-to-achieve manipulation of single qubits, these operations represent the basic steps of any quantum algorithm.

Surface redox-active centres in transition-metal oxides play a key role in determining the efficacy of electrocatalysts. The extreme sensitivity of surface redox states to temperatures, to gas pressures and to electrochemical reaction conditions renders them difficult to investigate by conventional surface-science techniques. Here we report the direct observation of surface redox processes by surface-sensitive, operando X-ray absorption spectroscopy using thin-film iron and cobalt perovskite oxides as model electrodes for elevated-temperature oxygen incorporation and evolution reactions. In contrast to the conventional view that the transition metal cations are the dominant redox-active centres, we find that the oxygen anions near the surface are a significant redox partner to molecular oxygen due to the strong hybridization between oxygen 2 p and transition metal 3 d electronic states. We propose that a narrow electronic state of significant oxygen 2 p character near the Fermi level exchanges electrons with the oxygen adsorbates. This result highlights the importance of surface anion-redox chemistry in oxygen-deficient transition-metal oxides. Surface redox centres in metal oxides play a key role in catalytic performance, and the conventional view is that the transition-metal cations dominate this behaviour. Here, the authors perform an in operando spectroscopic study, and find that oxygen anions are a significant redox partner to molecular oxygen.

One fundamental requirement for quantum computation is to carry out universal manipulations of quantum bits at rates much faster than the qubit’s rate of decoherence. Recently, fast gate operations have been demonstrated in logical spin qubits composed of two electron spins where the rapid exchange of the two electrons permits electrically controllable rotations around one axis of the qubit. However, universal control of the qubit requires arbitrary rotations around at least two axes. Here, we show that by subjecting each electron spin to a magnetic field of different magnitude, we achieve full quantum control of the two-electron logical spin qubit with nanosecond operation times. Using a single device, a magnetic-field gradient of several hundred millitesla is generated and sustained using dynamic nuclear polarization of the underlying Ga and As nuclei. Universal control of the two-electron qubit is then demonstrated using quantum state tomography. The presented technique provides the basis for single- and potentially multiple-qubit operations with gate times that approach the threshold required for quantum error correction. The spin state of two electrons in a double well is a promising qubit. Now, such qubits can be arbitrarily rotated around two different axes by applying a magnetic field of different magnitude to each electron. This can be done in nanoseconds, before the stored information is lost.

Long-ranged coherent qubit coupling is a missing function block for scaling up spin qubit based quantum computing solutions. Spin-coherent conveyor-mode electron-shuttling could enable spin quantum-chips with scalable and sparse qubit-architecture. Its key feature is the operation by only few easily tuneable input terminals and compatibility with industrial gate-fabrication. Single electron shuttling in conveyor-mode in a 420 nm long quantum bus has been demonstrated previously. Here we investigate the spin coherence during conveyor-mode shuttling by separation and rejoining an Einstein-Podolsky-Rosen (EPR) spin-pair. Compared to previous work we boost the shuttle velocity by a factor of 10000. We observe a rising spin-qubit dephasing time with the longer shuttle distances due to motional narrowing and estimate the spin-shuttle infidelity due to dephasing to be 0.7% for a total shuttle distance of nominal 560 nm. Shuttling several loops up to an accumulated distance of 3.36 μm, spin-entanglement of the EPR pair is still detectable, giving good perspective for our approach of a shuttle-based scalable quantum computing architecture in silicon. Electron charge and spin shuttling is a promising technique for connecting distant spin qubits. Here the authors use conveyor-mode shuttling to achieve high-fidelity transport of a single electron spin in Si/SiGe by separation and rejoining of two spin-entangled electrons across a shuttling distance of 560 nm.

The connectivity within single carrier information-processing devices requires transport and storage of single charge quanta. Single electrons have been adiabatically transported while confined to a moving quantum dot in short, all-electrical Si/SiGe shuttle device, called quantum bus (QuBus). Here we show a QuBus spanning a length of 10 μm and operated by only six simply-tunable voltage pulses. We introduce a characterization method, called shuttle-tomography, to benchmark the potential imperfections and local shuttle-fidelity of the QuBus. The fidelity of the single-electron shuttle across the full device and back (a total distance of 19 μm) is (99.7 ± 0.3) %. Using the QuBus, we position and detect up to 34 electrons and initialize a register of 34 quantum dots with arbitrarily chosen patterns of zero and single-electrons. The simple operation signals, compatibility with industry fabrication and low spin-environment-interaction in 28 Si/SiGe, promises long-range spin-conserving transport of spin qubits for quantum connectivity in quantum computing architectures. Electron spin qubits in SiGe dots have emerged as promising candidates for quantum information processing. Here the authors demonstrate conveyor-mode single electron shuttling in a Si/SiGe quantum dot device spanning the length of 10 micrometres and operated with a small number of controls

Quantum processor architectures must enable scaling to large qubit numbers while providing two-dimensional qubit connectivity and exquisite operation fidelities. For microwave-controlled semiconductor spin qubits, dense arrays have made considerable progress, but are still limited in size by wiring fan-out and exhibit significant crosstalk between qubits. To overcome these limitations, we introduce the SpinBus architecture, which uses electron shuttling to connect qubits and features low operating frequencies and enhanced qubit coherence. Device simulations for all relevant operations in the Si/SiGe platform validate the feasibility with established semiconductor patterning technology and operation fidelities exceeding 99.9%. Control using room temperature instruments can plausibly support at least 144 qubits, but much larger numbers are conceivable with cryogenic control circuits. Building on the theoretical feasibility of high-fidelity spin-coherent electron shuttling as key enabling factor, the SpinBus architecture may be the basis for a spin-based quantum processor that meets the scalability requirements for practical quantum computing. Semiconductor qubit architectures based on direct qubit coupling suffer from wiring fan-out and crosstalk as they scale up. Here the authors propose an architecture based on conveyor-mode shuttling of electron spins that tackles these issues and validate it numerically on quantum dot spin qubits in Si/SiGe.

Graphitic overlayers on metals have commonly been considered as inhibitors for surface reactions due to their chemical inertness and physical blockage of surface active sites. In this work, however, we find that surface reactions, for instance, CO adsorption/desorption and CO oxidation, can take place on Pt(111) surface covered by monolayer graphene sheets. Surface science measurements combined with density functional calculations show that the graphene overlayer weakens the strong interaction between CO and Pt and, consequently, facilitates the CO oxidation with lower apparent activation energy. These results suggest that interfaces between graphitic overlayers and metal surfaces act as 2D confined nanoreactors, in which catalytic reactions are promoted. The finding contrasts with the conventional knowledge that graphitic carbon poisons a catalyst surface but opens up an avenue to enhance catalytic performance through coating of metal catalysts with controlled graphitic covers. Significance Carbon deposits have been widely observed on metal surfaces in a variety of catalytic reactions, and the graphitic carbon species are often considered as inhibitors for surface reactions. We demonstrate here that CO adsorption and oxidation can occur on Pt surface covered by monolayer graphene, showing that the space between graphene overlayer and metal surface can act as a two-dimensional (2D) nanoreactor. Inside, CO oxidation happens with lower activation barrier due to the confinement effect of the graphene cover. This finding reminds us to reconsider the role of graphitic carbon in metal-catalyzed surface reactions and further provides a way to design novel catalysts.

Small spin-qubit registers defined by single electrons confined in Si/SiGe quantum dots operate successfully and connecting these would permit scalable quantum computation. Shuttling the qubit carrying electrons between registers is a natural choice for high-fidelity coherent links provided the overhead of control signals stays moderate. Our proof-of-principle demonstrates shuttling of a single electron by a propagating wave-potential in an electrostatically defined 420 nm long Si/SiGe quantum-channel. This conveyor-mode shuttling approach requires independent from its length only four sinusoidal control signals. We discuss the tuning of the signal parameters, detect the smoothness of the electron motion enabling the mapping of potential disorder and observe a high single-electron shuttling fidelity of 99.42 ± 0.02% including a reversal of direction. Our shuttling device can be readily embedded in industrial fabrication of Si/SiGe qubit chips and paves the way to solving the signal-fanout problem for a fully scalable semiconductor quantum-computing architecture.

Elastic strain is being increasingly employed to enhance the catalytic properties of mixed ion–electron conducting oxides. However, its effect on oxygen storage capacity is not well established. Here, we fabricate ultrathin, coherently strained films of CeO 2-δ between 5.6% biaxial compression and 2.1% tension. In situ ambient pressure X-ray photoelectron spectroscopy reveals up to a fourfold enhancement in equilibrium oxygen storage capacity under both compression and tension. This non-monotonic variation with strain departs from the conventional wisdom based on a chemical expansion dominated behaviour. Through depth profiling, film thickness variations and a coupled photoemission–thermodynamic analysis of space-charge effects, we show that the enhanced reducibility is not dominated by interfacial effects. On the basis of ab initio calculations of oxygen vacancy formation incorporating defect interactions and vibrational contributions, we suggest that the non-monotonicity arises from the tetragonal distortion under large biaxial strain. These results may guide the rational engineering of multilayer and core–shell oxide nanomaterials. The surface oxygen storage capacity is an important metric of catalytic activity, but its dependence on strain is not well characterized. Here, the authors show the surface oxygen nonstoichiometry in coherently strained CeO2-δ films increases non-monotonically with biaxial strain.