TGZ Molpro

Molpro 是一个全面的从头开始程序系统，用于高级分子电子结构计算，由 H.-J. 设计和维护。Werner 和 P. J. Knowles，并包含许多其他作者的贡献。 它包括用于标准计算化学应用的高效且并行化的程序，例如具有大量泛函选择的 DFT，以及最先进的高级耦合簇和多参考波函数方法。 电子激发态可以使用 MCSCF/CASSCF、CASPT2、MRCI 或 FCI 方法，或通过 TDDFT、CC2 和 EOM-CCSD 等响应方法进行处理。有许多模块用于 计算分子特性、几何优化、谐波和非谐波振动频率的计算，以及进一步的波函数分析。 分析能量梯度可用于 DFT、HF、MP2、MP2-F12、CCSD、CCSD-F12、DCSD、QCISD、QCISD（T）、CASSCF 和 CASPT2。密度拟合（DF 或 RI）近似可以加快具有大基集的 DFT 和 MP2 计算速度，具体如下： 数量级和显式相关方法 [MP2-F12、CCSD（T）-F12、CASPT2-F12、MRCI-F12] 最大限度地减少了基集不完备性误差，从而通过三重 zeta 基集产生接近 CBS 质量的结果。结合局部近似和高效并行化， 高级方法[PNO-LMP2-F12，PNO-LCCSD（T）-F12]可以应用于具有化学目的的大分子，从而产生前所未有的准确性（有关最近的综述，请参阅WIREs Comput Mol Sci. 2018，e1371）。 此外，WF-in-DFT包埋或QM/MM方法可用于将从头开始方法的适用性扩展到具有化学或生化兴趣的大型系统。

Molpro is a comprehensive system of ab initio programs for advanced molecular electronic structure calculations, designed and maintained by H.-J. Werner and P. J. Knowles, and containing contributions from many other authors. It comprises efficient and well parallelized programs for standard computational chemistry applications, such as DFT with a large choice of functionals, as well as state-of-the art high-level coupled-cluster and multi-reference wave function methods. Electronically excited states can be treated using MCSCF/CASSCF, CASPT2, MRCI, or FCI methods, or by response methods such as TDDFT, CC2, and EOM-CCSD. There are many modules for computing molecular properties, geometry optimization, calculation of harmonic and anharmonic vibrational frequencies, and further wave function analysis. Analytical energy gradients are available for DFT, HF, MP2, MP2-F12, CCSD, CCSD-F12, DCSD, QCISD, QCISD(T), CASSCF, and CASPT2. Density fitting (DF or RI) approximations can speed up DFT and MP2 calculations with large basis sets by orders of magnitude, and explicitly correlated methods [MP2-F12, CCSD(T)-F12, CASPT2-F12, MRCI-F12] minimize basis set incompleteness errors to yield near CBS quality results with triple-zeta basis sets. Combined with local approximations and efficient parallelizations, high-level methods [PNO-LMP2-F12, PNO-LCCSD(T)-F12] can be be applied to large molecules of chemical interest, yielding unprecedented accuracy (for a recent review see WIREs Comput Mol Sci. 2018, e1371). Furthermore, WF-in-DFT embedding or QM/MM methods can be used to extend the applicability of ab initio methods to large systems of chemical or biochemical interest.