Accurate Machine Learning Interatomic Potentials for Polyacene Molecular Crystals: Application to Single Molecule Host-Guest Systems
多并苯分子晶体的精确机器学习原子间势:应用于单分子主客体系统
Burak Gurlek, Shubham Sharma, Paolo Lazzaroni, Angel Rubio, Mariana Rossi
AI总结 利用基于图神经网络的MACE架构和主动学习策略,开发了适用于萘、蒽、并四苯和并五苯等多并苯分子晶体的通用机器学习原子间势,准确捕捉振动动力学,并用于研究主客体系统中的振动耦合。
详情
- Journal ref
- npj Comput Mater 11, 318 (2025)
新兴的机器学习原子间势(MLIPs)为大规模精确材料模拟提供了有前景的解决方案,但针对分子晶体中振动动力学描述的严格测试仍然稀缺。在这里,我们利用基于图神经网络的MACE架构和主动学习策略,开发了一个通用的MLIP,以准确捕捉一系列基于多并苯的分子晶体(即萘、蒽、并四苯和并五苯)的振动动力学。通过仔细的误差传播,我们表明这些势能是准确的,并能够研究非谐振动特征、振动寿命和振动耦合。特别是,我们研究了基于这些分子晶体的大规模主客体系统,展示了基于分子动力学技术解释和量化主体与客体核运动之间振动耦合的能力。我们的结果为理解大规模复杂分子系统中的振动特征建立了一个框架,从而代表了在分子环境中工程化振动相互作用的重要一步。
Emerging machine learning interatomic potentials (MLIPs) offer a promising solution for large-scale accurate material simulations, but stringent tests related to the description of vibrational dynamics in molecular crystals remain scarce. Here, we develop a general MLIP by leveraging the graph neural network-based MACE architecture and active-learning strategies to accurately capture vibrational dynamics across a range of polyacene-based molecular crystals, namely naphthalene, anthracene, tetracene and pentacene. Through careful error propagation, we show that these potentials are accurate and enable the study of anharmonic vibrational features, vibrational lifetimes, and vibrational coupling. In particular, we investigate large-scale host-guest systems based on these molecular crystals, showing the capacity of molecular-dynamics-based techniques to explain and quantify vibrational coupling between host and guest nuclear motion. Our results establish a framework for understanding vibrational signatures in large-scale complex molecular systems and thus represent an important step for engineering vibrational interactions in molecular environments.