Chemical tuning of quantum spin–electric coupling in molecular magnets

Controlling quantum spins using electric rather than magnetic fields promises substantial architectural advantages for developing quantum technologies. In this context, spins in molecular magnets offer tunability of spin-electric couplings (SECs) by rational chemical design. Here we demonstrate systematic control of SECs in a family of Mn(II)-containing molecules by varying the coordination environment of the spin centre. The trigonal bipyramidal (tbp) molecular structure with C3 symmetry leads to a substantial molecular electric dipole moment that is directly connected to its magnetic anisotropy. The interplay between these two features gives rise to experimentally observed SECs, which can be rationalized by wavefunction theoretical calculations. Our findings guide strategies for the development of electrically controllable molecular spin qubits for quantum technologies.