Experimental observation of spin defects in van der Waals material GeS$_2$

Abstract: Spin defects in atomically thin two-dimensional (2D) materials such as hexagonal boron nitride (hBN) attract significant attention for their potential quantum applications. The layered host materials not only facilitate seamless integration with optoelectronic devices but also enable the formation of heterostructures with on-demand functionality. Furthermore, their atomic thickness renders them particularly suitable for sensing applications. However, the short coherence times of the spin defects in hBN limit them in quantum applications that require extended coherence time. One primary reason is that both boron and nitrogen atoms have non-zero nuclear spins. Here, we present another 2D material germanium disulfide ($\beta$-GeS$2$) characterized by a wide bandgap and potential nuclear-spin-free lattice. This makes it as a promising host material for spin defects that possess long-coherence time. Our findings reveal the presence of more than two distinct types of spin defects in single-crystal $\beta$-GeS$_2$. Coherent control of one type defect has been successfully demonstrated at both 5 K and room temperature, and the coherence time $T_2$ can achieve tens of microseconds, 100-folds of that of negatively charged boron vacancy (V${\text{B}}^-$) in hBN, satisfying the minimal threshold required for metropolitan quantum networks--one of the important applications of spins. We entatively assign the observed optical signals come from substitution defects. Together with previous theoretical prediction, we believe the coherence time can be further improved with optimized lattice quality, indicating $\beta$-GeS$_2$ as a promising host material for long-coherence-time spins.