Developing molecular spin-optical functionality for quantum sensing

As exemplified by semiconductor-based defects, optically addressable spins are appealing platforms for quantum sensing. For such applications, there is a balance between optimising quantum properties (which thrive away from external influences) with the desire to efficiently couple to targets of interest (which favours close proximity to, and strong interactions with, the system of interest). With their nanoscale modularity, atomistic tunability, and scope for bottom-up assembly, molecular spin systems could provide an appealing balance of such features. However, a challenge for molecular spins has been achieving comparable spin-optical functionality to semiconductor-based defects. In this talk, we will describe our efforts to demonstrate and understand spin-optical functionality in molecular systems including room-temperature optically detected coherent manipulation of electron and nuclear spins, optically interfaced ground-state spins, and optically addressable spins in self-assembled architectures [1-6].

[1] PRL 133, 120801 (2024); [2] JACS 147, 22911 (2025); [3] arXiv:2610.17050; [4] MRS Bulletin 51, 312 (2026); [5] arXiv:2609.16851; [6] JACS 148, 44541 (2026)