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Hexagonal boron nitride (hBN) is a remarkable two-dimensional (2D) material that hosts solid-state spins and has great potential to be used in quantum information applications, including quantum networks. However, in this application, both the optical and spin properties are crucial for single spins but have not yet been discovered simultaneously for hBN spins. Here, we realize an efficient method for arraying and isolating the single defects of hBN and use this method to discover a new spin defect with a high probability of 85%. This single defect exhibits outstanding optical properties and an optically controllable spin, as indicated by the observed significant Rabi oscillation and Hahn echo experiments at room temperature. First principles calculations indicate that complexes of carbon and oxygen dopants may be the origin of the single spin defects. This provides a possibility for further addressing spins that can be optically controlled., 10 pages, 5 figures

Optically addressable spins in two-dimensional hexagonal boron nitride (hBN) attract widespread attention for their potential advantage in on-chip quantum devices, such as quantum sensors and quantum network. A variety of spin defects have been found in hBN, but no convenient and deterministic generation methods have been reported for other defects except negatively charged boron vacancy ($V_B^-$). Here we report that by using femtosecond laser direct writing technology, we can deterministically create spin defect ensembles with spectra range from 550 nm to 800 nm on nanoscale hBN flakes. Positive single-peak optically detected magnetic resonance (ODMR) signals are detected in the presence of magnetic field perpendicular to the substrate, and the contrast can reach 0.8%. With the appropriate thickness of hBN flakes, substrate and femtosecond laser pulse energy, we can deterministically and efficiently generate bright spin defect array. Our results provide a convenient deterministic method to create spin defects in hBN, which will motivate more endeavors for future researches and applications of spin-based technologies such as quantum magnetometer array.

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.

Quantum technology grown out of quantum information theory, including quantum communication, quantum computation and quantum sensing, not only provides powerful research tools for numerous fields, but also is expected to go to civilian use in the future. Solid-state spin-active defects are one of promising platforms for quantum technology, and the host materials include three-dimensional diamond and silicon carbide, and the emerging two-dimensional hexagonal boron nitride (hBN) and transition-metal dichalcogenides. In this review, we will focus on the spin defects in hBN, and summarize theoretical and experimental progresses made in understanding properties of these spin defects. In particular, the combination of theoretical prediction and experimental verification is highlighted. We also discuss the future advantages and challenges of solid-state spins in hBN on the path towards quantum information applications.

Two-dimensional hexagonal boron nitride (hBN) has attracted large attentions as platforms for realizations for integrated nanophotonics and collective effort has been focused on the spin defect centers. Here, the temperature dependence of the resonance spectrum in the range of 5-600 K is investigated. The zero-field splitting (ZFS) parameter D is found to decrease monotonicly with increasing temperature and can be described by Varshni empirical equation perfectly, while E almost does not change. We systematically study the differences among different hBN nanopowders and provide an evidence of edge effects on ODMR of VB- defects. Considering the proportional relation between D and reciprocal of lattice volume, the thermal expansion might be the dominant reason for energy-level shifts. We also demonstrate that the VB- defects still exist stably at least at 600 K. Moreover, we propose a scheme for detecting laser intensity using the VB- defects in hBN nanopowders, which is based on the obvious dependence of its D value on laser intensity. Our results are helpful to gain insight into the spin properties of VB- and for the realizations of miniaturized, integrated thermal sensor.