原子中心轨道数值框架下耦合团簇恒等解析方法的大规模并行实现
Massive-parallel Implementation of the Resolution-of-Identity Coupled-cluster Approaches in the Numeric Atom-centered Orbital Framework for Molecular Systems
摘要：
我们提出了一个双重并行实现的分辨率的身份（RI）耦合簇的方法，包括单，双和微扰三重激发，即RI-CCSD（T），在FHI-aims包的分子系统。在MPI/OpenMP混合框架中设计了一种基于域的分布式内存算法，有效地利用了内存带宽，并显著地减少了互连通信，特别是在计算粒子-粒子阶梯项时的张量收缩.我们的实现具有严格避免动态磁盘存储和出色的强大扩展到10，000个或更多核心的特点。以一组不同大小的分子为例，我们证明了我们的CCSD（T）代码的并行性能与最先进的高性能计算（HPC）计算化学软件包中的CC实现具有竞争力。我们还证明了在我们的RI-CCSD（T）中由于使用RI近似而引起的数值误差是可以忽略不计的。与相关一致的数值原子中心轨道（NAO）基组，NAO-VCC-nZ一起，该方法被应用于产生精确的理论参考数据的22个生物导向的弱相互作用（S22），11个气态半胱氨酸构象的构象能（CYCONF），和32异构化能（ISO 32）。
英文摘要：
We present a massive-parallel implementation of the resolution-of-identity (RI) coupled-cluster approach that includes single, double and perturbatively triple excitations, namely RI-CCSD(T), in the FHI-aims package for molecular systems. A domain-based distributed-memory algorithm in the MPI/OpenMP hybrid framework has been designed to effectively utilize the memory bandwidth and significantly minimize the interconnect communication, particularly for the tensor contraction in the evaluation of the particle-particle ladder term. Our implementation features a rigorous avoidance of the on-the-fly disk storage and an excellent strong scaling up to 10,000 and more cores. Taking a set of molecules with different sizes, we demonstrate that the parallel performance of our CCSD(T) code is competitive with the CC implementations in state-of-the-art high-performance computing (HPC) computational chemistry packages. We also demonstrate that the numerical error due to the use of RI approximation in our RI-CCSD(T) is negligibly small. Together with the correlation-consistent numeric atom-centered orbital (NAO) basis sets, NAO-VCC-nZ, the method is applied to produce accurate theoretical reference data for 22 bio-oriented weak interactions (S22), 11 conformational energies of gaseous cysteine conformers (CYCONF), and 32 isomerization energies (ISO32).
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