We demonstrated our ability to tune the spin and optical properties of a series of chromium (IV)aryl and alkyl compounds through atomistically precise chemical synthesis methods in collaboration with the Freedman Group. We designed a series of molecular complexes with spin-photon interfaces and ground state zero field splitting values addressable at readily available microwave frequencies. We showed that the ligand field of the molecular complexes has a significant impact on the electronic structure, modifying both the ground-state spin structure and the excited-state energy manifold, key aspects of resonant optical initialization and readout. Electron spin resonance and optical spectroscopy experiments were combined with theoretical calculations to show how chemical synthesis can be leveraged to tune spin and optical properties of these molecular systems, making them a versatile platform with possible applications in quantum sensing, computing and communication.

To learn more, please see: D. W. Laorenza, A. Kairalapova, S. L. Bayliss, T. Goldzak, S. M. Greene, L. R. Weiss, P. Deb, P. J. Mintun, K. A. Collins, D. D. Awschalom, T. C. Berkelbach, and D. E. Freedman, Journal of the American Chemical Society 143, 21350 (2021).