Qudit-Based Spectroscopy for Measurement and Control of Nuclear-Spin Qubits in Silicon Carbide.

Nuclear spins with hyperfine coupling to single electron spins are highly valuable quantum bits. Here we probe and characterize the particularly rich nuclear-spin environment around single silicon vacancy color centers (V2) in 4H-SiC. By using the electron spin-3/2 qudit as a four level sensor, we identify several sets of ^{29}Si and ^{13}C nuclear spins through their hyperfine interaction. We extract the major components of their hyperfine coupling via optical detected nuclear magnetic resonance, and assign them to shells in the crystal via the density function theory simulations. We utilize the ground-state level anticrossing of the electron spin for dynamic nuclear polarization and achieve a nuclear-spin polarization of up to 98±6%. We show that this scheme can be used to detect the nuclear magnetic resonance signal of individual spins and demonstrate their coherent control. Our work provides a detailed set of parameters and first steps for future use of SiC as a multiqubit memory and quantum computing platform.

First-principles theory of the nitrogen interstitial in hBN: a plausible model for the blue emitter.

Color centers in hexagonal boron nitride (hBN) have attracted considerable attention due to their remarkable optical properties enabling robust room temperature photonics and quantum optics applications in the visible spectral range. On the other hand, identification of the microscopic origin of color centers in hBN has turned out to be a great challenge that hinders the in-depth theoretical characterization, on-demand fabrication, and development of integrated photonic devices. This is also true for the blue emitter, which is a result of irradiation damage in hBN, emitting at 436 nm wavelength with desirable properties. Here, we propose the negatively charged nitrogen split interstitial defect in hBN as a plausible microscopic model for the blue emitter. To this end, we carried out a comprehensive first-principles theoretical study of the nitrogen interstitial. We carefully analyzed the accuracy of first-principles methods and showed that the commonly used HSE hybrid exchange-correlation functional fails to describe the electronic structure of this defect. Using the generalized Koopman's theorem, we fine-tuned the functional and obtained a zero-phonon photoluminescence (ZPL) energy in the blue spectral range. We showed that the defect exhibits a high emission rate in the ZPL line and features a characteristic phonon side band that resembles the blue emitter's spectrum. Furthermore, we studied the electric field dependence of the ZPL and numerically showed that the defect exhibits a quadratic Stark shift that is perpendicular to plane electric fields, making the emitter insensitive to electric field fluctuations in the first order. Our work emphasizes the need for assessing the accuracy of common first-principles methods in hBN and exemplifies a workaround methodology. Furthermore, our work is a step towards understanding the structure of the blue emitter and utilizing it in photonics applications.

Coherent dynamics of multi-spin V[Formula: see text] center in hexagonal boron nitride.

Hexagonal boron nitride (hBN) has recently been demonstrated to contain optically polarized and detected electron spins that can be utilized for implementing qubits and quantum sensors in nanolayered-devices. Understanding the coherent dynamics of microwave driven spins in hBN is of crucial importance for advancing these emerging new technologies. Here, we demonstrate and study the Rabi oscillation and related phenomena of a negatively charged boron vacancy (V[Formula: see text]) spin ensemble in hBN. We report on different dynamics of the V[Formula: see text] spins at weak and strong magnetic fields. In the former case the defect behaves like a single electron spin system, while in the latter case it behaves like a multi-spin system exhibiting multiple-frequency dynamical oscillation as beat in the Ramsey fringes. We also carry out theoretical simulations for the spin dynamics of V[Formula: see text] and reveal that the nuclear spins can be driven via the strong electron nuclear coupling existing in V[Formula: see text] center, which can be modulated by the magnetic field and microwave field.

Carbon defect qubit in two-dimensional WS2.

Identifying and fabricating defect qubits in two-dimensional semiconductors are of great interest in exploring candidates for quantum information and sensing applications. A milestone has been recently achieved by demonstrating that single defect, a carbon atom substituting sulphur atom in single layer tungsten disulphide, can be engineered on demand at atomic size level precision, which holds a promise for a scalable and addressable unit. It is an immediate quest to reveal its potential as a qubit. To this end, we determine its electronic structure and optical properties from first principles. We identify the fingerprint of the neutral charge state of the defect in the scanning tunnelling spectrum. In the neutral defect, the giant spin-orbit coupling mixes the singlet and triplet excited states with resulting in phosphorescence at the telecom band that can be used to read out the spin state, and coherent driving with microwave excitation is also viable. Our results establish a scalable qubit in a two-dimensional material with spin-photon interface at the telecom wavelength region.

Room-temperature control and electrical readout of individual nitrogen-vacancy nuclear spins.

Nuclear spins in semiconductors are leading candidates for future quantum technologies, including quantum computation, communication, and sensing. Nuclear spins in diamond are particularly attractive due to their long coherence time. With the nitrogen-vacancy (NV) centre, such nuclear qubits benefit from an auxiliary electronic qubit, which, at cryogenic temperatures, enables probabilistic entanglement mediated optically by photonic links. Here, we demonstrate a concept of a microelectronic quantum device at ambient conditions using diamond as wide bandgap semiconductor. The basic quantum processor unit - a single 14N nuclear spin coupled to the NV electron - is read photoelectrically and thus operates in a manner compatible with nanoscale electronics. The underlying theory provides the key ingredients for photoelectric quantum gate operations and readout of nuclear qubit registers. This demonstration is, therefore, a step towards diamond quantum devices with a readout area limited by inter-electrode distance rather than by the diffraction limit. Such scalability could enable the development of electronic quantum processors based on the dipolar interaction of spin-qubits placed at nanoscopic proximity.

DMRG on Top of Plane-Wave Kohn-Sham Orbitals: A Case Study of Defected Boron Nitride.

In this paper, we analyze the numerical aspects of the inherent multireference density matrix renormalization group (DMRG) calculations on top of the periodic Kohn-Sham density functional theory using the complete active space approach. The potential of the framework is illustrated by studying hexagonal boron nitride nanoflakes embedding a charged single boron vacancy point defect by revealing a vertical energy spectrum with a prominent multireference character. We investigate the consistency of the DMRG energy spectrum from the perspective of sample size, basis size, and active space selection protocol. Results obtained from standard quantum chemical atom-centered basis calculations and plane-wave based counterparts show excellent agreement. Furthermore, we also discuss the spectrum of the periodic sheet which is in good agreement with extrapolated data of finite clusters. These results pave the way toward applying the DMRG method in extended correlated solid-state systems, such as point defect qubit in wide band gap semiconductors.

Electrically driven optical interferometry with spins in silicon carbide.

Interfacing solid-state defect electron spins to other quantum systems is an ongoing challenge. The ground-state spin's weak coupling to its environment not only bestows excellent coherence properties but also limits desired drive fields. The excited-state orbitals of these electrons, however, can exhibit stronger coupling to phononic and electric fields. Here, we demonstrate electrically driven coherent quantum interference in the optical transition of single, basally oriented divacancies in commercially available 4H silicon carbide. By applying microwave frequency electric fields, we coherently drive the divacancy's excited-state orbitals and induce Landau-Zener-Stückelberg interference fringes in the resonant optical absorption spectrum. In addition, we find remarkably coherent optical and spin subsystems enabled by the basal divacancy's symmetry. These properties establish divacancies as strong candidates for quantum communication and hybrid system applications, where simultaneous control over optical and spin degrees of freedom is paramount.

Stabilization of point-defect spin qubits by quantum wells.

Defect-based quantum systems in wide bandgap semiconductors are strong candidates for scalable quantum-information technologies. However, these systems are often complicated by charge-state instabilities and interference by phonons, which can diminish spin-initialization fidelities and limit room-temperature operation. Here, we identify a pathway around these drawbacks by showing that an engineered quantum well can stabilize the charge state of a qubit. Using density-functional theory and experimental synchrotron X-ray diffraction studies, we construct a model for previously unattributed point defect centers in silicon carbide as a near-stacking fault axial divacancy and show how this model explains these defects' robustness against photoionization and room temperature stability. These results provide a materials-based solution to the optical instability of color centers in semiconductors, paving the way for the development of robust single-photon sources and spin qubits.

Hybrid-DFT + V w method for band structure calculation of semiconducting transition metal compounds: the case of cerium dioxide.

Hybrid functionals' non-local exchange-correlation potential contains a derivative discontinuity that improves on standard semi-local density functional theory (DFT) band gaps. Moreover, by careful parameterization, hybrid functionals can provide self-interaction reduced description of selected states. On the other hand, the uniform description of all the electronic states of a given system is a known drawback of these functionals that causes varying accuracy in the description of states with different degrees of localization. This limitation can be remedied by the orbital dependent exact exchange extension of hybrid functionals; the hybrid-DFT + V w method (Ivády et al 2014 Phys. Rev. B 90 035146). Based on the analogy of quasi-particle equations and hybrid-DFT single particle equations, here we demonstrate that parameters of hybrid-DFT + V w functional can be determined from approximate theoretical quasi-particle spectra without any fitting to experiment. The proposed method is illustrated on the charge self-consistent electronic structure calculation for cerium dioxide where itinerant valence states interact with well-localized 4f atomic like states, making this system challenging for conventional methods, either hybrid-DFT or LDA + U, and therefore allowing for a demonstration of the advantages of the proposed scheme.

Erratum: High-Fidelity Bidirectional Nuclear Qubit Initialization in SiC [Phys. Rev. Lett. 117, 220503 (2016)].

This corrects the article DOI: 10.1103/PhysRevLett.117.220503.

High-Fidelity Bidirectional Nuclear Qubit Initialization in SiC.

Dynamic nuclear polarization (DNP) is an attractive method for initializing nuclear spins that are strongly coupled to optically active electron spins because it functions at room temperature and does not require strong magnetic fields. In this Letter, we theoretically demonstrate that DNP, with near-unity polarization efficiency, can be generally realized in weakly coupled electron spin-nuclear spin systems. Furthermore, we theoretically and experimentally show that the nuclear spin polarization can be reversed by magnetic field variations as small as 0.8 Gauss. This mechanism offers new avenues for DNP-based sensors and radio-frequency free control of nuclear qubits.

Optical Polarization of Nuclear Spins in Silicon Carbide.

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 that we observe at room temperature corresponds to an effective nuclear temperature of 5 µK. 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.

Electrically and mechanically tunable electron spins in silicon carbide color centers.

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.

Asymmetric split-vacancy defects in SiC polytypes: a combined theoretical and electron spin resonance study.

Transition metal defects were studied in different polytypes of silicon carbide (SiC) by ab initio supercell calculations. We found asymmetric split-vacancy (ASV) complexes for these defects that preferentially form at only one site in hexagonal polytypes, and they may not be detectable at all in cubic polytype. Electron spin resonance study demonstrates the existence of ASV complex in niobium doped 4H polytype of SiC.