Rossi Mariana
Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761 Hamburg, Germany.
J Chem Phys. 2021 May 7;154(17):170902. doi: 10.1063/5.0042572.
Atomistic simulations based on the first-principles of quantum mechanics are reaching unprecedented length scales. This progress is due to the growth in computational power allied with the development of new methodologies that allow the treatment of electrons and nuclei as quantum particles. In the realm of materials science, where the quest for desirable emergent properties relies increasingly on soft weakly bonded materials, such methods have become indispensable. In this Perspective, an overview of simulation methods that are applicable for large system sizes and that can capture the quantum nature of electrons and nuclei in the adiabatic approximation is given. In addition, the remaining challenges are discussed, especially regarding the inclusion of nuclear quantum effects (NQEs) beyond a harmonic or perturbative treatment, the impact of NQEs on electronic properties of weakly bonded systems, and how different first-principles potential energy surfaces can change the impact of NQEs on the atomic structure and dynamics of weakly bonded systems.
基于量子力学第一原理的原子模拟正达到前所未有的长度尺度。这一进展得益于计算能力的提升以及新方法的发展，这些新方法允许将电子和原子核视为量子粒子进行处理。在材料科学领域，对理想涌现特性的追求越来越依赖于软的弱键合材料，此类方法已变得不可或缺。在此观点文章中，给出了适用于大系统规模且能在绝热近似下捕捉电子和原子核量子性质的模拟方法综述。此外，还讨论了尚存的挑战，特别是关于超出谐波或微扰处理范围纳入核量子效应（NQEs）、NQEs对弱键合系统电子性质的影响，以及不同的第一性原理势能面如何改变NQEs对弱键合系统原子结构和动力学的影响。
