Tailor-made force fields for crystal-structure prediction

被引:128
作者
Neumann, Marcus A. [1 ]
机构
[1] Avant Garde Mat Simulat, F-78100 St Germain En Laye, France
关键词
D O I
10.1021/jp710575h
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 general procedure is presented to derive a complete set of force-field parameters for flexible molecules in the crystalline state on a case-by-case basis. The force-field parameters are fitted to the electrostatic potential as well as to accurate energies and forces generated by means of a hybrid method that combines solid-state density functional theory (DFT) calculations with an empirical van der Waals correction. All DFT calculations are carried out with the VASP program. The mathematical structure of the force field, the generation of reference data, the choice of the figure of merit, the optimization algorithm, and the parameter-refinement strategy are discussed in detail. The approach is applied to cyclohexane-1,4-dione, a small flexible ring. The tailor-made force field obtained for cyclohexane-1,4-dione is used to search for low-energy crystal packings in all 230 space groups with one molecule per asymmetric unit, and the most stable crystal structures are reoptimized in a second step with the hybrid method. The experimental crystal structure is found as the most stable predicted crystal structure both with the tailor-made force field and the hybrid method. The same methodology has also been applied successfully to the four compounds of the fourth CCDC blind test on crystal-structure prediction. For the five aforementioned compounds, the root-mean-square deviations between lattice energies calculated with the tailor-made force fields and the hybrid method range from 0.024 to 0.053 kcal/mol per atom around an average value of 0.034 kcal/mol per atom.
引用
收藏
页码:9810 / 9829
页数:20
相关论文
共 28 条
[1]   Comparison of static and fluctuating charge models for force-field methods applied to organic crystals [J].
Brodersen, S ;
Wilke, S ;
Leusen, FJJ ;
Engel, GE .
CRYSTAL GROWTH & DESIGN, 2005, 5 (03) :925-933
[2]   A study of different approaches to the electrostatic interaction in force field methods for organic crystals [J].
Brodersen, S ;
Wilke, S ;
Leusen, FJJ ;
Engel, G .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2003, 5 (21) :4923-4931
[3]  
CORNELL WD, 1995, J AM CHEM SOC, V117, P5197
[4]   Beyond the isotropic atom model in crystal structure prediction of rigid molecules: Atomic multipoles versus point charges [J].
Day, GM ;
Motherwell, WDS ;
Jones, W .
CRYSTAL GROWTH & DESIGN, 2005, 5 (03) :1023-1033
[5]   A third blind test of crystal structure prediction [J].
Day, GM ;
Motherwell, WDS ;
Ammon, HL ;
Boerrigter, SXM ;
Della Valle, RG ;
Venuti, E ;
Dzyabchenko, A ;
Dunitz, JD ;
Schweizer, B ;
van Eijck, BP ;
Erk, P ;
Facelli, JC ;
Bazterra, VE ;
Ferraro, MB ;
Hofmann, DWM ;
Leusen, FJJ ;
Liang, C ;
Pantelides, CC ;
Karamertzanis, PG ;
Price, SL ;
Lewis, TC ;
Nowell, H ;
Torrisi, A ;
Scheraga, HA ;
Arnautova, YA ;
Schmidt, MU ;
Verwer, P .
ACTA CRYSTALLOGRAPHICA SECTION B-STRUCTURAL SCIENCE CRYSTAL ENGINEERING AND MATERIALS, 2005, 61 :511-527
[6]   ENERGY FUNCTIONS FOR PEPTIDES AND PROTEINS .1. DERIVATION OF A CONSISTENT FORCE-FIELD INCLUDING HYDROGEN-BOND FROM AMIDE CRYSTALS [J].
HAGLER, AT ;
HULER, E ;
LIFSON, S .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1974, 96 (17) :5319-5327
[7]   REPRESENTATION OF VANDERWAALS (VDW) INTERACTIONS IN MOLECULAR MECHANICS FORCE-FIELDS - POTENTIAL FORM, COMBINATION RULES, AND VDW PARAMETERS [J].
HALGREN, TA .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1992, 114 (20) :7827-7843
[8]   Energy minimization of crystal structures containing flexible molecules [J].
Karamertzanis, Panagiotis G. ;
Price, Sarah L. .
JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 2006, 2 (04) :1184-1199
[9]   AB-INITIO MOLECULAR-DYNAMICS SIMULATION OF THE LIQUID-METAL AMORPHOUS-SEMICONDUCTOR TRANSITION IN GERMANIUM [J].
KRESSE, G ;
HAFNER, J .
PHYSICAL REVIEW B, 1994, 49 (20) :14251-14269
[10]   Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set [J].
Kresse, G ;
Furthmuller, J .
PHYSICAL REVIEW B, 1996, 54 (16) :11169-11186