基于哈密顿量插值的通用量子炼金自由能模拟
General Quantum Alchemical Free Energy Simulations via Hamiltonian Interpolation
AI总结：
本文提出通过直接插值电子哈密顿量实现量子力学层面的炼金自由能模拟，兼容任意电子结构理论且每步仅需一次量子计算，并通过气相分子自由能变化和溶剂化分子pKa计算验证了方法的正确性与适用性。
摘要：
我们提出了一种在量子力学层面上通过直接插值电子哈密顿量来实现炼金自由能模拟的方法。该方法与任何电子结构理论级别兼容，并且每个分子动力学步骤仅需一次量子计算，而插值基态能量时则需要多次能量评估。我们通过计算气相分子的炼金自由能变化（包括原子核和电子的产生/湮灭）证明了该技术的正确性和适用性。我们还展示了对溶剂化分子的第一性原理pKa计算的初步应用，其中我们以量子力学方式湮灭了一个键合质子。
英文摘要：
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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