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We theoretically study the Hilbert space structure of two neighbouring Pdonor electrons in silicon-based quantum computer architectures. To useelectron spins as qubits, a crucial condition is the isolation of the electronspins from their environment, including the electronic orbital degrees offreedom. We provide detailed electronic structure calculations of both thesingle donor electron wave function and the two-electron pair wave function. Weadopted a molecular orbital method for the two-electron problem, forming abasis with the calculated single donor electron orbitals. Our two-electronbasis contains many singlet and triplet orbital excited states, in addition tothe two simple ground state singlet and triplet orbitals usually used in theHeitler-London approximation to describe the two-electron donor pair wavefunction. We determined the excitation spectrum of the two-donor system, andstudy its dependence on strain, lattice position and inter donor separation.This allows us to determine how isolated the ground state singlet and tripletorbitals are from the rest of the excited state Hilbert space. In addition tocalculating the energy spectrum, we are also able to evaluate the exchangecoupling between the two donor electrons, and the double occupancy probabilitythat both electrons will reside on the same P donor. These two quantities arevery important for logical operations in solid-state quantum computing devices,as a large exchange coupling achieves faster gating times, whilst the magnitudeof the double occupancy probability can affect the error rate.Comment: 15 pages (2-column

Molecular orbital calculations of two-electron states for P-donor solid-state spin qubits