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Abstract Point defect qubits in semiconductors have demonstrated their outstanding capabilities for high spatial resolution sensing generating broad multidisciplinary interest. Hexagonal boron nitride (hBN) hosting point defect qubits have recently opened up new horizons for quantum sensing by implementing sensing foils. The sensitivity of point defect sensors in hBN is currently limited by the linewidth of the magnetic resonance signal, which is broadened due to strong hyperfine couplings. Here, we report on a vacancy-related spin qubit with an inherently low symmetry configuration, the VB2 center, giving rise to a reduced magnetic resonance linewidth at zero magnetic fields. The VB2 centermore » is also equipped with a classical memory that can be utilized for storing population information. Using scanning transmission electron microscopy imaging, we confirm the existence of the VB2 configuration in free-standing monolayer hBN.« less

We demonstrate detection and measurement of electron paramagnetic spin resonances (EPR) of iron defects in $\beta \text{−}{\mathrm{Ga}}_2{\mathrm{O}}_3$ 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 ${45}^{\circ }$ 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 ${\mathrm{Fe}}^{3more »}$ + simultaneously. We confirm that ferric ${\mathrm{Fe}}^{3+}$ 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. Published by the American Physical Society 2024« less

Abstract Point defect quantum bits in semiconductors have the potential to revolutionize sensing at atomic scales. Currently, vacancy-related defects are at the forefront of high spatial resolution and low-dimensional sensing. On the other hand, it is expected that impurity-related defect structures may give rise to new features that could further advance quantum sensing in low dimensions. Here, we study the symmetric carbon tetramer clusters in hexagonal boron nitride and propose them as spin qubits for sensing. We utilize periodic-DFT and quantum chemistry approaches to reliably and accurately predict the electronic, optical, and spin properties of the studied defect. We showmore » that the nitrogen-centered symmetric carbon tetramer gives rise to spin state-dependent optical signals with strain-sensitive intersystem crossing rates. Furthermore, the weak hyperfine coupling of the defect to their spin environments results in a reduced electron spin resonance linewidth that can enhance sensitivity.« less

In this paper, we analyze the numerical aspects of the inherent multi reference 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 basedmore » 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.« less

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 roommore » 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.« less

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 findmore » 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.« less