Correction for dispersion and Coulombic interactions in molecular clusters with density functional derived methods: Application to polycyclic aromatic hydrocarbon clusters

被引:92
作者
Rapacioli, Mathias [1 ,2 ]
Spiegelman, Fernand [1 ,2 ]
Talbi, Dahbia [3 ]
Mineva, Tzonka [4 ]
Goursot, Annick [4 ]
Heine, Thomas [5 ]
Seifert, Gotthard [6 ]
机构
[1] Univ Toulouse, Lab Chim & Phys Quant, IRSAMC, UPS, F-31062 Toulouse, France
[2] CNRS, F-31062 Toulouse, France
[3] Univ Montpellier 2, GRAAL, CNRS UMR 5024, F-34095 Montpellier, France
[4] Ecole Chim Montpellier, Inst Gerhardt, UMR CNRS 5253, F-34296 Montpellier, France
[5] Jacobs Univ Bremen, Sch Sci & Engn, D-28759 Bremen, Germany
[6] Tech Univ Dresden, D-01062 Dresden, Germany
关键词
density functional theory; molecular clusters; molecular electronic states; organic compounds; potential energy functions; quasimolecules; SCF calculations; IV CHARGE MODEL; POTENTIAL-ENERGY SURFACE; PARTIAL ATOMIC CHARGES; DER-WAALS COMPLEXES; SCC-DFTB METHOD; BENZENE DIMER; INTERMOLECULAR INTERACTIONS; AB-INITIO; NONCOVALENT INTERACTIONS; THERMOCHEMICAL KINETICS;
D O I
10.1063/1.3152882
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 density functional based tight binding (DFTB) is a semiempirical method derived from the density functional theory (DFT). It inherits therefore its problems in treating van der Waals clusters. A major error comes from dispersion forces, which are poorly described by commonly used DFT functionals, but which can be accounted for by an a posteriori treatment DFT-D. This correction is used for DFTB. The self-consistent charge (SCC) DFTB is built on Mulliken charges which are known to give a poor representation of Coulombic intermolecular potential. We propose to calculate this potential using the class IV/charge model 3 definition of atomic charges. The self-consistent calculation of these charges is introduced in the SCC procedure and corresponding nuclear forces are derived. Benzene dimer is then studied as a benchmark system with this corrected DFTB (c-DFTB-D) method, but also, for comparison, with the DFT-D. Both methods give similar results and are in agreement with references calculations (CCSD(T) and symmetry adapted perturbation theory) calculations. As a first application, pyrene dimer is studied with the c-DFTB-D and DFT-D methods. For coronene clusters, only the c-DFTB-D approach is used, which finds the sandwich configurations to be more stable than the T-shaped ones.
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页数:10
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共 119 条
  • [1] Bader R. F. W., 1994, ATOMS MOL QUANTUM TH
  • [2] A WELL-BEHAVED ELECTROSTATIC POTENTIAL BASED METHOD USING CHARGE RESTRAINTS FOR DERIVING ATOMIC CHARGES - THE RESP MODEL
    BAYLY, CI
    CIEPLAK, P
    CORNELL, WD
    KOLLMAN, PA
    [J]. JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (40) : 10269 - 10280
  • [3] A density-functional model of the dispersion interaction
    Becke, AD
    Johnson, ER
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2005, 123 (15)
  • [4] Analysis of the emission of very small dust particles from Spitzer spectro-imagery data using blind signal separation methods
    Berne, O.
    Joblin, C.
    Deville, Y.
    Smith, J. D.
    Rapacioli, M.
    Bernard, J. P.
    Thomas, J.
    Reach, W.
    Abergel, A.
    [J]. ASTRONOMY & ASTROPHYSICS, 2007, 469 (02) : 575 - 586
  • [5] New exchange-correlation density functionals: The role of the kinetic-energy density
    Boese, AD
    Handy, NC
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2002, 116 (22) : 9559 - 9569
  • [6] The calculation of small molecular interactions by the differences of separate total energies. Some procedures with reduced errors (Reprinted from Molecular Physics, vol 19, pg 553-566, 1970)
    Boys, SF
    Bernardi, F
    [J]. MOLECULAR PHYSICS, 2002, 100 (01) : 65 - 73
  • [7] A second-generation reactive empirical bond order (REBO) potential energy expression for hydrocarbons
    Brenner, DW
    Shenderova, OA
    Harrison, JA
    Stuart, SJ
    Ni, B
    Sinnott, SB
    [J]. JOURNAL OF PHYSICS-CONDENSED MATTER, 2002, 14 (04) : 783 - 802
  • [8] CHARMM - A PROGRAM FOR MACROMOLECULAR ENERGY, MINIMIZATION, AND DYNAMICS CALCULATIONS
    BROOKS, BR
    BRUCCOLERI, RE
    OLAFSON, BD
    STATES, DJ
    SWAMINATHAN, S
    KARPLUS, M
    [J]. JOURNAL OF COMPUTATIONAL CHEMISTRY, 1983, 4 (02) : 187 - 217
  • [9] Density functional theory optimized basis sets for gradient corrected functionals:: 3d transition metal systems
    Calaminici, Patrizia
    Janetzko, Florian
    Koster, Andreas M.
    Mejia-Olvera, Roberto
    Zuniga-Gutierrez, Bernardo
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2007, 126 (04)
  • [10] CALVO F, ATOMIC MODELLING CLU