Electronic Structure and Coherence Properties of Molecular Color Centers from First Principles

We investigate the electronic and coherence properties of molecular complexes with a central spin-bearing metal ion coordinated to surrounding ligands [1]; these complexes allow for optical initialization and read out, together with as coherent microwave manipulation of the ground-state spin [1]. Specifically, we discuss the engineering of coherence times by isotopic substitution using cluster correlation expansion methods with ab initio-derived parameters [2,3] and the tuning of electronic properties by ligand engineering.<br/><br/>[1] S.L.Bayliss, D.W. Laorenza et al, Science 370, 1309; D.W. Laorenza et al. JACS 143, 50, 2021; S.L.Bayliss, P.Deb et al, PRX 12, 031028, 2022.<br/>[2] M. Onizhuk, G. Galli Adv. Theory Simul. 2100254, 2021<br/>[3] M. Onizhuk, G. Galli, https://arxiv.org/abs/2405.18535