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

共 69 条

[1] Approximating quantum many-body intermolecular interactions in molecular clusters using classical polarizable force fields [J].

Beran, Gregory J. O. .

JOURNAL OF CHEMICAL PHYSICS, 2009, 130 (16)

[2] Ab initio investigation of intermolecular interactions in solid benzene [J].

Bludsky, O. ;

Rubes, M. ;

Soldan, P. .

PHYSICAL REVIEW B, 2008, 77 (09)

[3] CALCULATION OF SMALL MOLECULAR INTERACTIONS BY DIFFERENCES OF SEPARATE TOTAL ENERGIES - SOME PROCEDURES WITH REDUCED ERRORS [J].

BOYS, SF ;

BERNARDI, F .

MOLECULAR PHYSICS, 1970, 19 (04) :553-&

[4] Enthalpies of sublimation of organic and organometallic compounds. 1910-2001 [J].

Chickos, JS ;

Acree, WE .

JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 2002, 31 (02) :537-698

[5] B3LYP augmented with an empirical dispersion term (B3LYP-D*) as applied to molecular crystals [J].

Civalleri, Bartolomeo ;

Zicovich-Wilson, Claudio M. ;

Valenzano, Loredana ;

Ugliengo, Piero .

CRYSTENGCOMM, 2008, 10 (04) :405-410

[6] PS13:: An open-source ab initio electronic structure package [J].

Crawford, T. Daniel ;

Sherrill, C. David ;

Valeev, Edward F. ;

Fermann, Justin T. ;

King, Rollin A. ;

Leininger, Matthew L. ;

Brown, Shawn T. ;

Janssen, Curtis L. ;

Seidl, Edward T. ;

Kenny, Joseph P. ;

Allen, Wesley D. .

JOURNAL OF COMPUTATIONAL CHEMISTRY, 2007, 28 (09) :1610-1616

[7] Electrostatically embedded many-body correlation energy, with applications to the calculation of accurate second-order Moller-Plesset perturbation theory energies for large water clusters [J].

Dahlke, Erin E. ;

Truhlar, Donald G. .

JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 2007, 3 (04) :1342-1348

[8] Atomistic calculations of phonon frequencies and thermodynamic quantities for crystals of rigid organic molecules [J].

Day, GM ;

Price, SL ;

Leslie, M .

JOURNAL OF PHYSICAL CHEMISTRY B, 2003, 107 (39) :10919-10933

[9] THERMODYNAMIC PROPERTIES OF MOLECULAR ORGANIC-CRYSTALS CONTAINING NITROGEN, OXYGEN, AND SULFUR .1. VAPOR-PRESSURES AND ENTHALPIES OF SUBLIMATION [J].

DEWIT, HGM ;

VANMILTENBURG, JC ;

DEKRUIF, CG .

JOURNAL OF CHEMICAL THERMODYNAMICS, 1983, 15 (07) :651-663

[10] GAUSSIAN-BASIS SETS FOR USE IN CORRELATED MOLECULAR CALCULATIONS .1. THE ATOMS BORON THROUGH NEON AND HYDROGEN [J].

DUNNING, TH .

JOURNAL OF CHEMICAL PHYSICS, 1989, 90 (02) :1007-1023

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