Electronic spins in semiconductors have been used extensively to explore the limits of external control over quantum mechanical phenomena. A long-standing goal of this research has been to identify or develop robust quantum systems that can be easily manipulated, for future use in advanced information and communication technologies. Recently, a point defect in diamond known as the nitrogen-vacancy centre has attracted a great deal of interest because it possesses an atomic-scale electronic spin state that can be used as an individually addressable, solid-state quantum bit (qubit), even at room temperature. These exceptional quantum properties have motivated efforts to identify similar defects in other semiconductors, as they may offer an expanded range of functionality not available to the diamond nitrogen-vacancy centre. Notably, several defects in silicon carbide (SiC) have been suggested as good candidates for exploration, owing to a combination of computational predictions and magnetic resonance data. Here we demonstrate that several defect spin states in the 4H polytype of SiC (4H-SiC) can be optically addressed and coherently controlled in the time domain at temperatures ranging from 20 to 300 kelvin. Using optical and microwave techniques similar to those used with diamond nitrogen-vacancy qubits, we study the spin-1 ground state of each of four inequivalent forms of the neutral carbon-silicon divacancy, as well as a pair of defect spin states of unidentified origin. These defects are optically active near telecommunication wavelengths, and are found in a host material for which there already exist industrial-scale crystal growth and advanced microfabrication techniques. In addition, they possess desirable spin coherence properties that are comparable to those of the diamond nitrogen-vacancy centre. This makes them promising candidates for various photonic, spintronic and quantum information applications that merge quantum degrees of freedom with classical electronic and optical technologies.

Identifying and designing physical systems for use as qubits, the basic units of quantum information, are critical steps in the development of a quantum computer. Among the possibilities in the solid state, a defect in diamond known as the nitrogen-vacancy (NV −1 ) center stands out for its robustness-its quantum state can be initialized, manipulated, and measured with high fidelity at room temperature. Here we describe how to systematically identify other deep center defects with similar quantum-mechanical properties. We present a list of physical criteria that these centers and their hosts should meet and explain how these requirements can be used in conjunction with electronic structure theory to intelligently sort through candidate defect systems. To illustrate these points in detail, we compare electronic structure calculations of the NV −1 center in diamond with those of several deep centers in 4H silicon carbide (SiC). We then discuss the proposed criteria for similar defects in other tetrahedrally coordinated semiconductors.semiconductor defects | spintronics | first-principles calculations A quantum computer is a device that would exploit the rules of quantum mechanics to solve certain computational problems more efficiently than allowed by Boolean logic (1). Over the past two decades, qubits have been implemented in a wide variety of materials, including atoms (2), liquids (3), and solids such as superconductors (4), semiconductors (5), and ion-doped insulators (6). Recently, the diamond nitrogen-vacancy (NV −1 ) center has emerged as a leading qubit candidate because it is an individually addressable quantum system that may be initialized, manipulated, and measured with high fidelity at room temperature (7). Interestingly, even though these successes stem largely from the defect's nature as a deep center (a point defect with highly localized electronic bound states confined to a region on the scale of a single lattice constant), no systematic effort has been made to identify other deep centers that might behave similarly. We outline the physical features that such deep centers and their hosts should exhibit and show how these criteria can be used to identify potential qubit candidates within a large class of defects structurally analogous to the diamond NV −1 . To aid in the illustration of these points, we compare density functional theory (DFT) calculations of the diamond NV −1 with those of several defects found in 4H-SiC.Searching for deep centers that behave like the diamond NV −1 is worthwhile for several reasons. From an engineering perspective, it is currently quite difficult to grow and fabricate devices from diamond. The discovery of a similar defect in a more technologically mature host material might allow for more sophisticated implementations of single-and multiqubit devices. Additionally, because deep centers and semiconductors as a whole exhibit a diverse set of physical characteristics, innovative areas of device functionality may potentially arise once the quantum properties of these...

Crystal defects can confine isolated electronic spins and are promising candidates for solid-state quantum information. Alongside research focusing on nitrogen-vacancy centres in diamond, an alternative strategy seeks to identify new spin systems with an expanded set of technological capabilities, a materials-driven approach that could ultimately lead to ‘designer’ spins with tailored properties. Here we show that the 4H, 6H and 3C polytypes of SiC all host coherent and optically addressable defect spin states, including states in all three with room-temperature quantum coherence. The prevalence of this spin coherence shows that crystal polymorphism can be a degree of freedom for engineering spin qubits. Long spin coherence times allow us to use double electron–electron resonance to measure magnetic dipole interactions between spin ensembles in inequivalent lattice sites of the same crystal. Together with the distinct optical and spin transition energies of such inequivalent states, these interactions provide a route to dipole-coupled networks of separately addressable spins.

The divacancies in SiC are a family of paramagnetic defects that show promise for quantum communication technologies due to their long-lived electron spin coherence and their optical addressability at near-telecom wavelengths. Nonetheless, a high-fidelity spin-photon interface, which is a crucial prerequisite for such technologies, has not yet been demonstrated. Here, we demonstrate that such an interface exists in isolated divacancies in epitaxial films of 3C-SiC and 4H-SiC. Our data show that divacancies in 4H-SiC have minimal undesirable spin mixing, and that the optical linewidths in our current sample are already similar to those of recent remote entanglement demonstrations in other systems. Moreover, we find that 3C-SiC divacancies have a millisecond Hahn-echo spin coherence time, which is among the longest measured in a naturally isotopic solid. The presence of defects with these properties in a commercial semiconductor that can be heteroepitaxially grown as a thin film on Si shows promise for future quantum networks based on SiC defects.

Funding Agencies|ARO [W911NF-15-2-0058]; AFOSR [FA9550-15-1-0029, FA9550-14-1-0231]; NSF MRSEC [DMR-1420709]; DOE LDRD Program; Swedish Research Council [621-2014-5825, 2016-04068]; AForsk foundation [16-576]; Carl-Trygger Stiftelse for Vetenskaplig Forskning [CTS 15:339]; Knut and Alice Wallenberg Foundation [KAW 2013.0300]; JSPS [26286047]; Swedish Energy Agency [43611-1]

The electron spins of semiconductor defects can have complex interactions with their host, particularly in polar materials like SiC where electrical and mechanical variables are intertwined. By combining pulsed spin resonance with ab initio simulations, we show that spin-spin interactions in 4H-SiC neutral divacancies give rise to spin states with a strong Stark effect, sub-10(-6) strain sensitivity, and highly spin-dependent photoluminescence with intensity contrasts of 15%-36%. These results establish SiC color centers as compelling systems for sensing nanoscale electric and strain fields

We demonstrate optically pumped dynamic nuclear polarization of 29 Si nuclear spins that are strongly coupled to paramagnetic color centers in 4H-and 6H-SiC. The 99 ± 1% degree of polarization at room temperature corresponds to an effective nuclear temperature of 5 K. By combining ab initio theory with the experimental identification of the color centers' optically excited states, we quantitatively model how the polarization derives from hyperfine-mediated level anticrossings. These results lay a foundation for SiC-based quantum memories, nuclear gyroscopes, and hyperpolarized probes for magnetic resonance imaging. Main text:Silicon carbide is a promising material for quantum electronics at the wafer scale. It is both amenable to sophisticated device processing [1] and a host for several types of vacancy-related paramagnetic color centers with remarkable attributes . Much like the diamond nitrogen-vacancy center [24, 25], these color centers localize electronic states that can exhibit millisecond-long spin coherence times [18], singlespin addressability through confocal optically detected magnetic resonance (ODMR) [18,19], and ODMR persistence up to room temperature [10,11,14,19]. Although fluctuating nuclear spins are a principal source of electronic spin decoherence [26], their presence is not purely detrimental. If polarized and controlled, nuclear spins in SiC would be a technologically important resource.In this Letter, we show that near-infrared light can nearly completely polarize populations of 29 Si nuclear spins in SiC. This process is based on dynamic nuclear polarization (DNP) [27,28]: the optically pumped polarization of of electron spins bound to either neutral divacancy [4,

The successful implementation of the nitrogen-vacancy (NV) center in diamond as a qubit has spawned a great deal of interest in this defect. In principle, similar defects suitable for quantum computing should exist in other material systems; however, very little work has been done on identifying NV-like centers in other materials. We discuss the key properties of the NV center in diamond in the context of uncovering similar defects in other materials, with the specific example of SiC. Using first-principles calculations, we compare the properties of the NV center in diamond to the analogous defect in 4H-SiC. We also compare the properties of the bare vacancies. We calculate defect formation energies and charge-state transition levels to determine which defects are likely to form. Then, by analyzing the defect-induced electronic states, we determine whether stable defects in 4H-SiC may have properties similar to those of the NV center in diamond.

Spins bound to point defects are increasingly viewed as an important resource for solid-state implementations of quantum information and spintronic technologies. In particular, there is a growing interest in the identification of new classes of defect spin that can be controlled optically. Here, we demonstrate ensemble optical spin polarization and optically detected magnetic resonance (ODMR) of the S = 1 electronic ground state of chromium (Cr 4+ ) impurities in silicon carbide (SiC) and gallium nitride (GaN). Spin polarization is made possible by the narrow optical linewidths of these ensembles (<8.5 GHz), which are similar in magnitude to the ground state zero-field spin splitting energies of the ions at liquid helium temperatures. This allows us to optically resolve individual spin sublevels within the ensembles at low magnetic fields using resonant excitation from a cavity-stabilized, narrow-linewidth laser. Additionally, these near-infrared emitters possess exceptionally weak phonon sidebands, ensuring that >73% of the overall optical emission is contained with the defects' zero-phonon lines. These characteristics make this semiconductor-based, transition metal impurity system a promising target for further study in the ongoing effort to integrate optically active quantum states within common optoelectronic materials.