发表机构
Sorbonne Université; CNRS; Physicochimie des Électrolytes et Nanosystèmes Interfaciaux; Réseau sur le Stockage Electrochimique de l’Energie (RS2E)（索邦大学; 法国国家科学研究中心; 界面电解质与纳米系统物理化学; 电化学储能网络）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本文深入分析了哈密顿自适应分辨率模拟（H-AdResS）方法在界面建模中热浴方案和长程静电模型选择的影响，指出Langevin热浴可靠而Nosé-Hoover产生伪影，短程静电模型导致非物理结果，并讨论了力与能量不连续性的截断策略及键合自由度插值的不可行性。
AI 中文摘要
哈密顿自适应分辨率模拟（H-AdResS）方法允许在单个模拟盒子中结合原子和基于粒子的粗粒度模型，这使得它对建模包含界面或反应区域且周围有相互作用环境的系统非常有吸引力。在我们之前的工作[ arXiv:2604.21867 ]中，我们在LAMMPS 2023中实现了H-AdResS，并将其应用扩展到界面，以MOF/CO$_2$界面为例。我们发现，尽管有这些优点，但正确使用该方法处理这类系统并非易事。本文深入分析了热浴方案和长程静电模型选择的影响。尽管其哈密顿公式允许在恒温系综中进行H-AdResS模拟，但并非所有热浴都适用。我们证明Langevin热浴是该方法的可靠选择，而Nosé-Hoover会导致伪影。此外，我们表明使用短程模型如阻尼位移力方法处理静电（这是H-AdResS模拟的常用选择）在建模界面时可能导致非物理结果。还讨论了处理由分辨率突变引起的力和能量不连续性所需的截断策略。最后，讨论了无法更改H-AdResS哈密顿定义以包含键合自由度逐渐插值的问题。我们希望本文能帮助读者正确设置H-AdResS模拟，并评估该方法是否能准确建模其感兴趣的系统。
英文摘要
The Hamiltonian-Adaptive Resolution Simulation (H-AdResS) method allows to combine atomistic and particle-based coarse-grained models in a single simulation box, which makes it very attractive to model systems containing interfaces or reactive regions surrounded by an interacting environment. In our previous work [J. Chem. Inf. Model. (2026) 66 (15): 9215-9225], we implemented H-AdResS in LAMMPS (2 Aug 2023 version) and extended its use to interfaces, focusing on MOF/CO$_2$ interfaces as an example. We found that, despite its advantages, using this method properly for this kind of systems is not trivial. In this work, an in-depth analysis of the impact of the choice of thermostatting schemes and long-range electrostatics models is presented. Even though its Hamiltonian formulation enables performing H-AdResS simulations within constant temperatures ensembles, not every thermostat is appropriate. We demonstrate that Langevin thermostat is a reliable choice for this method, while Nosé-Hoover results in artifacts. In addition, we show that using short-range models such as the Damped Shifted Force method for electrostatics, a popular choice for H-AdResS simulations, can lead to non-physical results when modeling interfaces. The need of capping strategies to deal with discontinuities in forces and energies arising from abrupt changes in resolution is also discussed. Finally, the impossibility of changing the definition of the H-AdResS Hamiltonian to include a gradual interpolation of the bonded degrees of freedom is discussed. We hope that this contribution helps the reader to appropriately set up H-AdResS simulations and to assess if this method can be used to accurately model their system of interest.
Comments21 pages, 19 figures
