Papers › General Quantum Alchemical Free Energy Simulations via Hamiltonian Interpolation

General Quantum Alchemical Free Energy Simulations via Hamiltonian Interpolation

30 Aug 2024arXiv:2408.17002links table onlyarchive 2025-07-28

Chenghan Li, Xing Zhang, Garnet Kin-Lic Chan

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We present an implementation of alchemical free energy simulations at the quantum mechanical level by directly interpolating the electronic Hamiltonian. The method is compatible with any level of electronic structure theory and requires only one quantum calculation for each molecular dynamics step in contrast to multiple energy evaluations that would be needed when interpolating the ground-state energies. We demonstrate the correctness and applicability of the technique by computing alchemical free energy changes of gas-phase molecules, with both nuclear and electron creation/annihilation. We also show an initial application to first-principles pKa calculation for solvated molecules where we quantum mechanically annihilate a bonded proton.

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