Detrimental Increase of Spin-Phonon Coupling in Molecular Qubits on Substrates

Molecular qubits are a promising platform for quantum information systems. Although single molecule and ensemble studies have assessed the performance of S= 1/2 molecules, it is understood that to function in devices, regular arrays of addressable qubits supported by a substrate are needed. The substrate imposes mechanical and electronic boundary conditions on the molecule; however, the impact of these effects on spin–lattice relaxation times is not well understood. Here we perform electronic structure calculations to assess the effects of a graphene (Cgr) substrate on the molecular qubit copper phthalocyanine (CuPc). We use a progressive Hessian approach to efficiently calculate and separate the substrate contributions. We also use a simple thermal model to predict the impact of these changes on the spin-phonon coupling from 0 to 200 K. Further analysis of the individual vibrational modes with and without Cgrshows that an overall increase in SPC between the vibrations modes of CuPc with the surface reduces the spin–lattice relaxation time T1. We explain these changes by examining how the substrate lifts symmetries of CuPc in the absorbed configuration. Our work shows that a surface can have a large unintentional impact on SPC and that ways to reduce this coupling need to be found to fully exploit arrays of molecular qubits in device architectures.