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. We elaborate on the methodology of computing color centers in periodic and cluster models of hBN. Using first-principles methods, we determined various optical properties of the nitrogen interstitial defect and compared them to experimental results.

We demonstrate detection and measurement of electron paramagnetic spin resonances (EPR) of iron defects in 𝛽−Ga2⁢O3 utilizing generalized ellipsometry at frequencies between 110 and 170 GHz. The experiments are performed on an Fe-doped single crystal in a free-beam configuration in reflection at 45∘ and magnetic fields between 3 and 7 T. In contrast with low-field, low-frequency EPR measurements, we observe all five transitions of the 𝑠=5/2 high-spin state Fe3+ simultaneously. We confirm that ferric Fe3+ is predominantly found at octahedrally coordinated Ga sites. We obtain the full set of fourth-order monoclinic zero-field splitting parameters for both octahedrally and tetrahedrally coordinated sites by employing measurements at multiple sample azimuth rotations. The capability of high-field EPR allows us to demonstrate that simplified second-order orthorhombic spin Hamiltonians are insufficient, and fourth-order terms as well as consideration of the monoclinic symmetry are needed. These findings are supported by computational approaches based on density-functional theory for second-order and on ligand-field theory for fourth-order parameters of the spin Hamiltonian. Terahertz ellipsometry is a way to measure spin resonances in a cavity-free setup. Its possibility of varying the probe frequency arbitrarily without otherwise changing the experimental setup offers unique means of truly disentangling different components of highly anisotropic spin Hamiltonians.

Hexagonal boron nitride (hBN) has recently gained attention as a solid state host of quantum emitters. In particular, the recently discovered B centers show promise for integration in scalable quantum technologies thanks to site-specific defect generation and a reproducible wavelength. Here we employ spectral hole burning spectroscopy and resonant polarization measurements to observe nearly coherent hBN quantum emitters, both as singles and in ensembles, with three discrete polarization axes indicative of a C (2v) symmetry defect. Our results constitute an important milestone toward the implementation of hBN quantum emitters in integrated quantum photonics.

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 Si29 and C13 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.

Defects in semiconductors have in recent years been revealed to have interesting properties in the venture towards quantum technologies. In this regard, silicon carbide has shown great promise as a host for quantum defects. In particular, the ultrabright AB photoluminescence lines in 4⁢H-Si⁢C are observable at room temperature and have been proposed as a single-photon quantum emitter. These lines have previously been studied and assigned to the carbon–antisite-vacancy (CAV) pair. In this paper, we report on new measurements of the AB lines’ temperature dependence, and carry out an in-depth computational study on the optical properties of the CAV defect. We find that the CAV defect has the potential to exhibit several different zero-phonon luminescences with emissions in the near-infrared telecom band, in its neutral and positive charge states. However, our measurements show that the AB lines only consist of three nonthermally activated lines instead of the previously reported four lines; meanwhile, our calculations on the CAV defect are unable to find optical transitions in full agreement with the AB-line assignment. In light of our results, the identification of AB lines and the associated room-temperature emission require further study.

The negatively charged silicon vacancy (V-Si(-)) in silicon carbide is a well-studied point defect for quantum applications. At the same time, a closer inspection of ensemble photoluminescence and electron paramagnetic resonance measurements reveals an abundance of related but so far unidentified signals. In this study, we search for defects in 4H-SiC that explain the above magneto-optical signals in a defect database generated by automatic defect analysis and qualification (ADAQ) workflows. This search reveals only one class of atomic structures that exhibit silicon-vacancy-like properties in the data: a carbon anti-site (C-Si) within sub-nanometer distances from the silicon vacancy only slightly alters the latter without affecting the charge or spin state. Such a perturbation is energetically bound. We consider the formation of V-Si(-) + C-Si; up to 2 nm distance and report their zero phonon lines and zero field splitting values. In addition, we perform high-resolution photoluminescence experiments in the silicon vacancy region and find an abundance of lines. Comparing our computational and experimental results, several configurations show great agreement. Our work demonstrates the effectiveness of a database with high-throughput results in the search for defects in quantum applications.

Automatic Defect Analysis and Qualification (ADAQ) is a collection of automatic workflows developed for high-throughput simulations of magneto-optical properties of point defects in semiconductors. These workflows handle the vast number of defects by automating the processes to relax the unit cell of the host material, construct supercells, create point defect clusters, and execute calculations in both the electronic ground and excited states. The main outputs are the magneto-optical properties which include zero-phonon lines, zero-field splitting, and hyperfine coupling parameters. In addition, the formation energies are calculated. We demonstrate the capability of ADAQ by performing a complete characterization of the silicon vacancy in silicon carbide in the polytype 4H (4H-SiC).

We investigated the structural and electrical properties of 2D MXene sheets by means of firstprinciples density functional theory (DFT) calculations. To describe the Kohn-Sham states, plane wave basis set and projector augmented wave method (PAW) were used as implemented in the Vienna ab initio Simulation Package (VASP). We applied PBE parameterization of the generalized gradient approximation of the exchange and correlation energy functional to account for many-body effects of the interacting electron system. Convergent sampling of the Brillouin-zone was achieved by a Γ-centered 15×15×1 grid. In order to model a single sheet of MXene we ensured at least 30 Å vacuum between the periodically repeated sheets. For the structural optimization 1×10−3 eV/Å force criteria was used. The relativistic spin-orbit coupling effects were also included in our simulations regarding band structure and density of states.

In n-type 4H-SiC grown by chemical vapor deposition and irradiated by low-energy (250 keV) electrons, an electron paramagnetic resonance center, labeled EI8a, was observed at room temperature. A short anneal at temperatures in the range of 300-500 °C in darkness changes EI8a to a new center, labeled EI8b, which can be converted back by illumination at room temperature. We show that EI8a and EI8b are the two different configurations of the same defect, labeled EI8, with C_1h symmetry and an electron spin S=1/2. The EI8 center is stable up to ~650 °C and annealed out at ~800 °C. Based on the observed hyperfine structures due to the hyperfine interaction between the electron spin and the nuclear spins of four ²⁹Si atoms and three ¹³C atoms, the EI8 center is suggested to be related to a carbon interstitial cluster.

We demonstrate optically pumped dynamic nuclear polarization of Si-29 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 mu 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.