Atomistic tight-binding Hartree-Fock calculations of multielectron configurations in P-doped silicon devices: Wavefunction reshaping

Donor-based quantum devices in silicon are attractive platforms for universal quantum computing and analog quantum simulations. The nearly atomic precision in dopant placement promises great control over the quantum properties of these devices. We present atomistic calculations and a detailed analysis of many-electron states in a single phosphorus atom and selected phosphorus dimers in silicon. Our self-consistent method involves atomistic calculations of the electron energies utilizing representative tight-binding Hamiltonians, computations of Coulomb and exchange integrals without any reference to an atomic orbital set, and solutions to the associated Hartree-Fock equations. First, we assess the quality of our tight-binding Hartree-Fock protocol against configuration-interaction calculations for two electrons in a single phosphorus atom, finding that our formalism provides an accurate estimation of the electron-electron repulsion energy requiring smaller computational boxes and self-consistent single-electron wavefunctions. Then, we compute charging and binding energies in phosphorus dimers observing their variation as a function of impurity-impurity separation. Our calculations predict an antiferromagnetic ground state for the two-electron system and a weakly bound three-electron state in the range of separations considered. We rationalize these results in terms of the single-electron energies, charging energies, and the wavefunction reshaping.