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Optically addressable spins in widebandgap semiconductors have become one ofthe most prominent platforms for exploring fundamental quantum phenomena. Whileseveral candidates in 3D crystals including diamond and silicon carbide havebeen extensively studied, the identification of spindependent processes inatomically thin 2D materials has remained elusive. Although opticallyaccessible spin states in hBN are theoretically predicted, they have not yetbeen observed experimentally. Here, employing rigorous electron paramagneticresonance techniques and photoluminescence spectroscopy, we identifyfluorescence lines in hexagonal boron nitride associated with a particulardefect, the negatively charged boron vacancy and determine the parameters ofits spin Hamiltonian. We show that the defect has a triplet ground state with azero field splitting of 3.5 GHz and establish that the centre exhibitsoptically detected magnetic resonance at room temperature. We also demonstratethe spin polarization of this centre under optical pumping, which leads tooptically induced population inversion of the spin ground state a prerequisitefor coherent spin manipulation schemes. Our results constitute a leap forwardin establishing two dimensional hBN as a prime platform for scalable quantumtechnologies, with extended potential for spin based quantum information andsensing applications, as our ODMR studies on hBN NV diamonds hybrid structuresshow.

Room Temperature Initialisation and Readout of Intrinsic Spin Defects in a Van der Waals Crystal