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Quantum defects are atomic defects in materials that provide resources to construct quantum information devices such as single-photon emitters and spin qubits. Recently, two-dimensional (2D) materials gained prominence as a host of quantum defects with many attractive features derived from their atomically thin and layered material formfactor. In this Perspective, we discuss first-principles computational methods and challenges to predict the spin and electronic properties of quantum defects in 2D materials. We focus on the open quantum system nature of the defects and their interaction with external parameters such as electric field, magnetic field, and lattice strain. We also discuss how such prediction and understanding can be used to guide experimental studies, ranging from defect identification to tuning of their spin and optical properties. This Perspective provides significant insights into the interplay between the defect, the host material, and the environment, which will be essential in the pursuit of ideal two-dimensional quantum defect platforms. 

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 ${\mathrm{Fe}}^{3+}$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 Society2024 

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.