Efficient Quantum Chemical Calculation of Structure Ensembles and Free Energies for Nonrigid Molecules

被引：134

作者：

Grimme, Stefan ^{[1
]}

Bohle, Fabian ^{[1
]}

Hansen, Andreas ^{[1
]}

Pracht, Philipp ^{[1
]}

Spicher, Sebastian ^{[1
]}

Stahn, Marcel ^{[1
]}

机构：

[1] Univ Bonn, Mulliken Ctr Theoret Chem, Inst Phys & Theoret Chem, D-53115 Bonn, Germany

来源：

JOURNAL OF PHYSICAL CHEMISTRY A | 2021年 / 125卷 / 19期

关键词：

DENSITY-FUNCTIONAL THEORY; HARMONIC VIBRATIONAL FREQUENCIES; SOLVATION FREE-ENERGIES; COMPUTATIONAL CHEMISTRY; PARTITION-COEFFICIENTS; NDDO APPROXIMATIONS; FLEXIBLE MOLECULES; AQUEOUS-SOLUTION; BINDING; PREDICTION;

D O I：

10.1021/acs.jpca.1c00971

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The application of quantum chemical, automatic multilevel modeling workflows for the determination of thermodynamic (e.g., conformation equilibria, partition coefficients, pK a values) and spectroscopic properties of relatively large, nonrigid molecules in solution is described. Key points are the computation of rather complete structure (conformer) ensembles with extremely fast but still reasonable GFN2-xTB or GFN-FF semiempirical methods in the CREST searching approach and subsequent refinement at a recently developed, accurate r(2)SCAN-3c DFT composite level. Solvation effects are included in all steps by accurate continuum solvation models (ALPB, (D)COSMO-RS). Consistent inclusion of thermostatistical contributions in the framework of the modified rigid-rotor-harmonic-oscillator approximation (mRRHO) based on xTB/FF computed PES is also recommended.

引用

页码：4039 / 4054

页数：16

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