Ab Initio Magneto-Optical Spectrum of Group-IV Vacancy Color Centers in Diamond

Group-IV vacancy color centers in diamond are fast emerging qubits that can be harnessed in quantum communication and sensor applications. There is an immediate quest for understanding their magneto-optical properties, in order to select the appropriate qubits for varying needs of particular quantum applications. Here we present results from cutting-edge ab initio calculations about the charge state stability, zero-phonon-line energies, and spin-orbit and electron-phonon couplings for group-IV vacancy color centers. Based on the analysis of our results, we develop a novel spin Hamiltonian for these qubits which incorporates the interaction of the electron spin and orbit coupled with phonons beyond perturbation theory. Our results are in good agreement with previous data and predict a new defect for qubit applications with thermally initialized ground state spin and long spin coherence time.