实时运动方程耦合簇累积量格林函数方法：基于张量代数的多体方法异构并行实现
Real-time Equation-of-Motion Coupled-Cluster Cumulant Green's Function Method: Heterogeneous Parallel Implementation Based on the Tensor Algebra for Many-body Methods Infrastructure
摘要：
我们报告了在多体方法张量代数（TAMM）基础设施中实现实时运动方程耦合簇（RT-EOM-CC）累积量格林函数方法[J. Chem. Phys. 152，174113（2020）]。TAMM是一个大规模并行异构张量库，旨在利用即将到来的exascale计算资源。两体电子排斥矩阵元的Cholesky分解，我们施加自旋显式形式的各种运营商时，评估张量收缩。与我们之前的实代数张量收缩引擎（TCE）实现不同，TAMM实现支持完全复杂的代数。使用一阶Adams-Moulton方法传播RT-EOM-CC单（S）和双（D）时间相关幅度。这种新的实现显示出出色的可扩展性测试高达500 GPU使用锌卟啉分子与655个基函数，与90%以上的并行效率高达400 GPU。利用TAMRT-EOM-CCSD研究了甲醛和三氟乙酸乙酯（ESCA）分子的芯光发射光谱。对后者的模拟涉及多达71个占据轨道和649个虚轨道。相对准粒子电离能和总的光谱函数与现有的实验结果符合得很好。
英文摘要：
We report the implementation of the real-time equation-of-motion coupled-cluster (RT-EOM-CC) cumulant Green's function method [J. Chem. Phys. 152, 174113 (2020)] within the Tensor Algebra for Many-body Methods (TAMM) infrastructure. TAMM is a massively parallel heterogeneous tensor library designed for utilizing forthcoming exascale computing resources. The two-body electron repulsion matrix elements are Cholesky-decomposed, and we imposed spin-explicit forms of the various operators when evaluating the tensor contractions. Unlike our previous real algebra Tensor Contraction Engine (TCE) implementation, the TAMM implementation supports fully complex algebra. The RT-EOM-CC singles (S) and doubles (D) time-dependent amplitudes are propagated using a first-order Adams--Moulton method. This new implementation shows excellent scalability tested up to 500 GPUs using the Zn-porphyrin molecule with 655 basis functions, with parallel efficiencies above 90\% up to 400 GPUs. The TAMM RT-EOM-CCSD was used to study core photo-emission spectra in the formaldehyde and ethyl trifluoroacetate (ESCA) molecules. Simulations of the latter involve as many as 71 occupied and 649 virtual orbitals. The relative quasiparticle ionization energies and overall spectral functions agree well with available experimental results.
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