非共价键相互作用的量子蒙特卡罗方法：一种达到基准精度的有效方法
Quantum Monte Carlo for Noncovalent Interactions: An Efficient Protocol Attaining Benchmark Accuracy
摘要：
非共价相互作用能的可靠理论预测在药物设计和储氢应用等方面很重要，属于当代量子化学的长期挑战。在这方面，固定节点扩散蒙特卡罗（FN-DMC）是一个很有前途的替代常用的“金标准”耦合集群CCSD（T）/CBS方法的基准精度和有利的缩放，在其他相关的波函数的方法相比。这项工作的重点是分析的协议和可能的权衡FN-DMC估计的非共价相互作用能，并提出了一个有效而准确的计算协议，使用简化的显式相关项与有利的O（N^3）标度。它与许多复合物的CCSD（T）/CBS数据实现了良好的一致性（平均无符号误差~0.2 kcal/mol），包括苯/氢、T形苯二聚体、堆叠的腺嘌呤-胸腺嘧啶和一组小的非共价复合物A24。CCSD（T）/CBS的高准确度和低计算成本决定了其在大非共价复合物的实际相互作用能计算中的应用。
英文摘要：
Reliable theoretical predictions of noncovalent interaction energies, which are important e.g. in drug-design and hydrogen-storage applications, belong to longstanding challenges of contemporary quantum chemistry. In this respect, the fixed-node diffusion Monte Carlo (FN-DMC) is a promising alternative to the commonly used "gold standard" coupled-cluster CCSD(T)/CBS method for its benchmark accuracy and favourable scaling, in contrast to other correlated wave function approaches. This work is focused on the analysis of protocols and possible tradeoffs for FN-DMC estimations of noncovalent interaction energies and proposes an efficient yet accurate computational protocol using simplified explicit correlation terms with a favorable O(N^3) scaling. It achieves an excellent agreement (mean unsigned error ~0.2 kcal/mol) with respect to the CCSD(T)/CBS data on a number of complexes, including benzene/hydrogen,T-shape benzene dimer, stacked adenine-thymine and a set of small noncovalent complexes A24. The high accuracy and reduced computational costs predestinate the reported protocol for practical interaction energy calculations of large noncovalent complexes, where the CCSD(T)/CBS is prohibitively expensive.
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