双生成跨轨道使显式相关的缩尺耦合簇方法既稳健又简单。
Geminal-spanning orbitals make explicitly correlated reduced-scaling coupled-cluster methods robust, yet simple.
作者信息
Pavošević Fabijan, Neese Frank, Valeev Edward F
机构信息
Department of Chemistry, Virginia Tech, Blacksburg, Virginia 24061, USA.
Max Planck Institut für Chemische Energiekonversion, Stiftstr. 34-36, D-45470 Mülheim an der Ruhr, Germany.
出版信息
J Chem Phys. 2014 Aug 7;141(5):054106. doi: 10.1063/1.4890002.
We present a production implementation of reduced-scaling explicitly correlated (F12) coupled-cluster singles and doubles (CCSD) method based on pair-natural orbitals (PNOs). A key feature is the reformulation of the explicitly correlated terms using geminal-spanning orbitals that greatly reduce the truncation errors of the F12 contribution. For the standard S66 benchmark of weak intermolecular interactions, the cc-pVDZ-F12 PNO CCSD F12 interaction energies reproduce the complete basis set CCSD limit with mean absolute error <0.1 kcal/mol, and at a greatly reduced cost compared to the conventional CCSD F12.
我们展示了一种基于对自然轨道（PNO）的缩尺显式相关（F12）耦合簇单双激发（CCSD）方法的生产实现。一个关键特性是使用双占据跨越轨道重新表述显式相关项，这极大地减少了F12贡献的截断误差。对于弱分子间相互作用的标准S66基准测试，cc-pVDZ-F12 PNO CCSD F12相互作用能以平均绝对误差<0.1 kcal/mol再现了完全基组CCSD极限，并且与传统的CCSD F12相比成本大幅降低。
Zotero 插件