Near-Frustration-Free Electronic Structure Hamiltonian Representations and Lower-Bound Certificates

Abstract Hamiltonian representations based on the sum-of-squares (SOS) hierarchy provide rigorous lower bounds on ground-state energies and facilitate the design of efficient classical and quantum simulation algorithms. This work presents a unified framework connecting SOS decompositions with variational two-particle reduced density matrix (v2RDM) theory. We demonstrate that the “weighted” SOS ansatz naturally recovers the dual of the v2RDM program, enabling the strict enforcement of symmetry constraints such as particle number and spin. We provide explicit SOS constructions for the Hubbard model and electronic structure Hamiltonians, ranging from spin-free approximations to full rank-2 expansions. We also highlight theoretical connections to block-invariant symmetry shifts. Numerical benchmarks on molecular systems and iron–sulfur clusters validate these near-frustration-free representations, demonstrating their utility in improving spectral gap amplification and reducing block-encoding costs in quantum algorithms.