Calculating spin dephasing in molecular spin systems using combined open systems and electronic structure methods

Understanding the spin dynamics of molecular spin systems is crucial to the engineering and design of molecular qubit candidates. Many open questions remain in connecting molecular geometry to spin dephasing times (T₂). Using Hamiltonians generated from electronic structure methods in conjunction with an open system framework allows the calculation of T₂ while considering the impact of important phenomena such as the spin diffusion barrier and the delocalization of spin on decoherence times. Understanding these contributions to T₂ could provide insight into the connection between molecular geometry and decoherence.