核-电子轨道子系统密度泛函理论
Nuclear-Electronic Orbital Subsystem Density Functional Theory
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中文总结 AI 辅助
研究提出NEO-sDFT方法，可对数千原子的大分子体系量子化学计算，误差仅几meV，计算标度良好，为生化体系质子转移模拟提供基础。
中文摘要 AI 辅助
我们提出一种基于核-电子轨道（NEO）和子系统密度泛函理论（sDFT）的新型计算方法。所得到的NEO-sDFT方法可对由数千个原子组成的大分子体系进行量子化学计算，同时对选定的质子进行量子力学描述。该程序实现的关键特性在于其在将量子质子分配至子系统时具有灵活性，允许在统一框架内采用不同的嵌入方案。通过计算水二聚体的相互作用能，评估了NEO-sDFT的准确性，与参考核-电子轨道密度泛函理论（NEO-DFT）结果相比，其误差仅为几meV。通过对尺寸递增的水团簇进行计算，进一步展示了NEO-sDFT良好的计算标度，其中多达303个质子被进行量子力学处理。我们的结果表明，NEO-sDFT是一种将核量子效应纳入大规模模拟的准确且高效的方法，为后续应用于生化体系中的质子转移过程奠定了基础。
英文摘要
We present a new computational approach based on Nuclear-Electronic Orbital and Subsystem Density Functional Theory. The resulting NEO-sDFT methodology enables quantum chemical calculations of large molecular systems composed of thousands of atoms while also describing selected protons quantum mechanically. A key feature of the associated program implementation is its flexibility in assigning quantum protons to subsystems, allowing different embedding schemes to be employed within a unified framework. The accuracy of NEO-sDFT is assessed by computing water dimer interaction energies, which exhibit errors of only a few meV compared to reference Nuclear-Electronic Orbital Density Functional Theory results. The favorable computational scaling of NEO-sDFT is further showcased through calculations on water clusters of increasing size, with up to 303 protons being treated quantum mechanically. Our results demonstrate that NEO-sDFT is an accurate and efficient approach for incorporating nuclear quantum effects into large-scale simulations, providing a foundation for future applications to proton transfer processes in biochemical systems.
