Predicting Organic Crystal Lattice Energies with Chemical Accuracy

被引：184

作者：

Beran, Gregory J. O. ^{[1
]}

Nanda, Kaushik ^{[1
]}

机构：

[1] Univ Calif Riverside, Dept Chem, Riverside, CA 92521 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2010年 / 1卷 / 24期

关键词：

DENSITY-FUNCTIONAL THEORY; PLESSET PERTURBATION-THEORY; QUANTUM-CHEMISTRY; COUPLED-CLUSTER; BASIS-SETS; MP2; MODEL; COMPUTATION; ENTHALPIES; COMPLEXES;

D O I：

10.1021/jz101383z

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：

A fast, fragment-based hybrid many-body interaction model is used to optimize the structures of five small-molecule organic crystals (with fixed experimental lattice parameters) and predict their lattice energies with accuracies of 2-4 kJ/mol compared to experiment. This model treats individual molecules in the central unit cell and their short-range two-body interactions quantum mechanically, while long-range electrostatics and many-body induction are treated with a classical polarizable force field. For the hydrogen bonded ice, formamide, and acetamide crystals, MP2 calculations extrapolated to the complete-basis-set limit provide good accuracy. However, MP2 exhibits difficulties for crystals such as benzene and imidazole, where pi-stacking dispersion interactions are important, and post-MP2 corrections determined from small-basis-set CCSD(T) calculations are required to achieve chemical accuracy. Using these techniques, accurate crystal lattice energy predictions for small-molecule organic crystals are feasible with currently available computing power.

引用

页码：3480 / 3487

页数：8

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