A major challenge in using spins in the solid state for quantum technologies is protecting them from sources of decoherence. This is particularly important in nanodevices where the proximity of material interfaces, and their associated defects, can play a limiting role. Spin decoherence can be addressed to varying degrees by improving material purity or isotopic composition, for example, or active error correction methods such as dynamic decoupling (or even combinations of the two). However, a powerful method applied to trapped ions in the context of atomic clocks is the use of particular spin transitions that are inherently robust to external perturbations. Here, we show that such 'clock transitions' can be observed for electron spins in the solid state, in particular using bismuth donors in silicon. This leads to dramatic enhancements in the electron spin coherence time, exceeding seconds. We find that electron spin qubits based on clock transitions become less sensitive to the local magnetic environment, including the presence of (29)Si nuclear spins as found in natural silicon. We expect the use of such clock transitions will be of additional significance for donor spins in nanodevices, mitigating the effects of magnetic or electric field noise arising from nearby interfaces and gates.

Spin defects in silicon carbide have exceptional electron spin coherence with a nearinfrared spin-photon interface in a material amenable to modern semiconductor fabrication. Leveraging these advantages, we successfully integrate highly coherent single neutral divacancy spins in commercially available p-i-n structures and fabricate diodes to modulate the local electrical environment of the defects. These devices enable deterministic charge state control and broad Stark shift tuning exceeding 850 GHz. Surprisingly, we show that charge depletion results in a narrowing of the optical linewidths by over 50 fold, approaching the lifetime limit. These results demonstrate a method for mitigating the ubiquitous problem of spectral diffusion in solid-state emitters by engineering the electrical environment while utilizing classical semiconductor devices to control scalable spin-based quantum systems.

Defects with associated electron and nuclear spins in solid-state materials have a long history relevant to quantum information science going back to the first spin echo experiments with silicon dopants in the 1950s. Since the turn of the century, the field has rapidly spread to a vast array of defects and host crystals applicable to quantum communication, sensing, and computing. From simple spin resonance to longdistance remote entanglement, the complexity of working with spin defects is fast advancing, and requires an in-depth understanding of their spin, optical, charge, and material properties in this modern context. This is especially critical for discovering new relevant systems dedicated to specific quantum applications. In this review, we therefore expand upon all the key components with an emphasis on the properties of defects and the host material, on engineering opportunities and other pathways for improvement. Finally, this review aims to be as defect and material agnostic as possible, with some emphasis on optical emitters, providing a broad guideline for the field of solid-state spin defects for quantum information.

Hybrid spin-mechanical systems provide a platform for integrating quantum registers and transducers. Efficient creation and control of such systems require a comprehensive understanding of the individual spin and mechanical components as well as their mutual interactions. Point defects in silicon carbide (SiC) offer long-lived, optically addressable spin registers in a wafer-scale material with low acoustic losses, making them natural candidates for integration with high quality factor mechanical resonators. Here, we show Gaussian focusing of a surface acoustic wave in SiC, characterized by a novel stroboscopic X-ray diffraction imaging technique, which delivers direct, strain amplitude information at nanoscale spatial resolution. Using ab initio calculations, we provide a more complete picture of spin-strain coupling for various defects in SiC with C 3v symmetry. This reveals the importance of shear for future device engineering and enhanced spin-mechanical coupling. We demonstrate all-optical detection of acoustic paramagnetic resonance without microwave magnetic fields, relevant to sensing applications. Finally, we show mechanically driven Autler-Townes splittings and magnetically forbidden Rabi oscillations. These results offer a basis for full strain control of three-level spin systems.

Solid-state quantum emitters with spin registers are promising platforms for quantum communication, yet few emit in the narrow telecom band necessary for low-loss fiber networks. Here, we create and isolate near-surface single vanadium dopants in silicon carbide (SiC) with stable and narrow emission in the O band, with brightness allowing cavity-free detection in a wafer-scale material. In vanadium ensembles, we characterize the complex d1 orbital physics in all five available sites in 4H-SiC and 6H-SiC. The optical transitions are sensitive to mass shifts from local silicon and carbon isotopes, enabling optically resolved nuclear spin registers. Optically detected magnetic resonance in the ground and excited orbital states reveals a variety of hyperfine interactions with the vanadium nuclear spin and clock transitions for quantum memories. Last, we demonstrate coherent quantum control of the spin state. These results provide a path for telecom emitters in the solid state for quantum applications.

Defects in silicon carbide (SiC) have emerged as a favorable platform for optically active spin-based quantum technologies. Spin qubits exist in specific charge states of these defects, where the ability to control these states can provide enhanced spin-dependent readout and long-term charge stability. We investigate this charge state control for two major spin qubits in 4H-SiC, the divacancy and silicon vacancy, obtaining bidirectional optical charge conversion between the bright and dark states of these defects. We measure increased photoluminescence from divacancy ensembles by up to three orders of magnitude using near-ultraviolet excitation, depending on the substrate, and without degrading the electron spin coherence time. This charge conversion remains stable for hours at cryogenic temperatures, allowing spatial and persistent patterning of the charge state populations. We develop a comprehensive model of the defects and optical processes involved, offering a strong basis to improve material design and to develop quantum applications in SiC.

The decoherence of mixed electron-nuclear spin qubits is a topic of great current importance, but understanding is still lacking: while important decoherence mechanisms for spin qubits arise from quantum spin bath environments with slow decay of correlations, the only analytical framework for explaining observed sharp variations of decoherence times with magnetic field is based on the suppression of classical noise. Here we obtain a general expression for decoherence times of the central spin system which exposes significant differences between quantum-bath decoherence and decoherence by classical field noise. We perform measurements of decoherence times of bismuth donors in natural silicon using both electron spin resonance (ESR) and nuclear magnetic resonance (NMR) transitions, and in both cases find excellent agreement with our theory across a wide parameter range. The universality of our expression is also tested by quantitative comparisons with previous measurements of decoherence around 'optimal working points' or 'clock transitions' where decoherence is strongly suppressed. We further validate our results by comparison to cluster expansion simulations.

We present a complete theoretical treatment of Stark effects in bulk doped silicon, whose predictions are supported by experimental measurements. A multi-valley effective mass theory, dealing non-perturbatively with valley-orbit interactions induced by a donor-dependent central cell potential, allows us to obtain a very reliable picture of the donor wave function within a relatively simple framework. Variational optimization of the 1s donor binding energies calculated with a new trial wave function, in a pseudopotential with two fitting parameters, allows an accurate match of the experimentally determined donor energy levels, while the correct limiting behavior for the electronic density, both close to and far from each impurity nucleus, is captured by fitting the measured contact hyperfine coupling between the donor nuclear and electron spin.We go on to include an external uniform electric field in order to model Stark physics: With no extra ad hoc parameters, variational minimization of the complete donor ground energy allows a quantitative description of the field-induced reduction of electronic density at each impurity nucleus. Detailed comparisons with experimental values for the shifts of the contact hyperfine coupling reveal very close agreement for all the donors measured (P, As, Sb and Bi). Finally, we estimate field ionization thresholds for the donor ground states, thus setting upper limits to the gate manipulation times for single qubit operations in Kane-like architectures: the Si:Bi system is shown to allow for A gates as fast as ≈10 MHz.