Rank-reduced coupled-cluster. III. Tensor hypercontraction of the doubles amplitudes
Rank-reduced coupled-cluster. III. Tensor hypercontraction of the doubles amplitudes
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DOI：
10.1063/5.0077770
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发表时间：
2022-02-07
影响因子：
4.4
通讯作者：
Martinez, Todd J.
中科院分区：
文献类型：
--
作者：
Hohenstein, Edward G.;Fales, B. Scott;Martinez, Todd J.
我们开发了一个四次标度实现耦合集群单和双打（CCSD）的基础上低秩张量超收缩（THC）因子分解的电子排斥积分（ERI）和双打振幅。这扩展了我们的降秩（RR）耦合簇方法，将高阶张量因子分解。双倍振幅的THC分解占了计算效率的大部分增益，因为它与ERI的Cholesky分解相结合足以降低CCSD振幅方程的大部分贡献的计算复杂性。进一步的THC因式分解的ERI减少了某些条款的复杂性所产生的双重激发运营商和双电子运营商之间的嵌套的recruitors。我们实现了这种新的算法，使用图形处理单元，并证明它使CCSD计算的分子与250个原子和2500个基础功能，使用一个单一的计算机节点。此外，我们表明，新的方法计算相关能量具有可比的准确性的基本RR-CCSD方法。
We develop a quartic-scaling implementation of coupled-cluster singles and doubles (CCSD) based on low-rank tensor hypercontraction (THC) factorizations of both the electron repulsion integrals (ERIs) and the doubles amplitudes. This extends our rank-reduced (RR) coupled-cluster method to incorporate higher-order tensor factorizations. The THC factorization of the doubles amplitudes accounts for most of the gain in computational efficiency as it is sufficient, in conjunction with a Cholesky decomposition of the ERIs, to reduce the computational complexity of most contributions to the CCSD amplitude equations. Further THC factorization of the ERIs reduces the complexity of certain terms arising from nested commutators between the doubles excitation operator and the two-electron operator. We implement this new algorithm using graphical processing units and demonstrate that it enables CCSD calculations for molecules with 250 atoms and 2500 basis functions using a single computer node. Furthermore, we show that the new method computes correlation energies with comparable accuracy to the underlying RR-CCSD method.