Department of Chemistry and the PULSE Institute, Stanford University, Stanford, California 94305, USA and SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
J Chem Phys. 2017 Oct 28;147(16):161723. doi: 10.1063/1.4997997.
Analytic energy gradients for tensor hyper-contraction (THC) are derived and implemented for second-order Møller-Plesset perturbation theory (MP2), with and without the scaled-opposite-spin (SOS)-MP2 approximation. By exploiting the THC factorization, the formal scaling of MP2 and SOS-MP2 gradient calculations with respect to system size is reduced to quartic and cubic, respectively. An efficient implementation has been developed that utilizes both graphics processing units and sparse tensor techniques exploiting spatial sparsity of the atomic orbitals. THC-MP2 has been applied to both geometry optimization and ab initio molecular dynamics (AIMD) simulations. The resulting energy conservation in micro-canonical AIMD demonstrates that the implementation provides accurate nuclear gradients with respect to the THC-MP2 potential energy surfaces.
分析张量高收缩（THC）的能量梯度，并为二阶 Møller-Plesset 微扰理论（MP2）及其带和不带标度相反自旋（SOS）-MP2 近似的情况实现这些梯度。通过利用 THC 分解，可以将 MP2 和 SOS-MP2 梯度计算的形式比例缩小到分别为四次和三次。开发了一种有效的实现方法，该方法同时利用图形处理单元和稀疏张量技术，利用原子轨道的空间稀疏性。THC-MP2 已应用于几何优化和从头分子动力学（AIMD）模拟。微正则 AIMD 中的能量守恒表明，该实现方法提供了 THC-MP2 势能表面的准确核梯度。
