Electric field sensitivity of molecular color centers

Molecular color centers with S=1 ground states are promising candidates for quantum sensing of electric fields. These molecules have an electronic structure similar to solid state color centers, but they allow for processing modalities that permit direct interfacing with an analyte. Currently, it is unknown how sensitive these molecules are to electric fields and what molecular properties affect their sensitivity. We perform density functional theory calculations to understand the impact of electric fields on the electronic structure of five nominally tetrahedral molecular color centers exhibiting variable transition metal chemistry and ligand densities. We then extract the Stark parameters from each of these molecules and compare them to molecular properties such as the dipole moment and inner shell stiffness and find that the dipole moment of the molecule largely governs sensitivity. We predict that polar heteroleptic molecules may have electric field sensitivities comparable to solid state color centers such as nitrogen-vacancy centers in diamond. (c) 2024 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution-NonCommercial 4.0International (CC BY-NC) license.