JCP Nameplate
  • Volume/Page
  • Keyword
  • DOI
  • Citation
  • Advanced
   
 
 
 

You Tube Flickr Twitter UniPHY Group iResearch App Facebook

Journal of Chemical Physics / Volume 132 / Issue 15 / ARTICLES / Theoretical Methods and Algorithms

J. Chem. Phys. 132, 154104 (2010); http://dx.doi.org/10.1063/1.3382344 (19 pages)

A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu

Stefan Grimme, Jens Antony, Stephan Ehrlich, and Helge Krieg

Theoretische Organische Chemie, Organisch-Chemisches Institut, Universität Münster, Corrensstrasse 40, D-48149 Münster, Germany

View MapView Map

(Received 18 January 2010; accepted 16 March 2010; published online 16 April 2010)

The method of dispersion correction as an add-on to standard Kohn–Sham density functional theory (DFT-D) has been refined regarding higher accuracy, broader range of applicability, and less empiricism. The main new ingredients are atom-pairwise specific dispersion coefficients and cutoff radii that are both computed from first principles. The coefficients for new eighth-order dispersion terms are computed using established recursion relations. System (geometry) dependent information is used for the first time in a DFT-D type approach by employing the new concept of fractional coordination numbers (CN). They are used to interpolate between dispersion coefficients of atoms in different chemical environments. The method only requires adjustment of two global parameters for each density functional, is asymptotically exact for a gas of weakly interacting neutral atoms, and easily allows the computation of atomic forces. Three-body nonadditivity terms are considered. The method has been assessed on standard benchmark sets for inter- and intramolecular noncovalent interactions with a particular emphasis on a consistent description of light and heavy element systems. The mean absolute deviations for the S22 benchmark set of noncovalent interactions for 11 standard density functionals decrease by 15%–40% compared to the previous (already accurate) DFT-D version. Spectacular improvements are found for a tripeptide-folding model and all tested metallic systems. The rectification of the long-range behavior and the use of more accurate C6 coefficients also lead to a much better description of large (infinite) systems as shown for graphene sheets and the adsorption of benzene on an Ag(111) surface. For graphene it is found that the inclusion of three-body terms substantially (by about 10%) weakens the interlayer binding. We propose the revised DFT-D method as a general tool for the computation of the dispersion energy in molecules and solids of any kind with DFT and related (low-cost) electronic structure methods for large systems.

© 2010 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. THEORY
    1. General
    2. Dispersion coefficients
    3. Three-body term
    4. Cutoff radii
    5. Coordination number dependent dispersion coefficients
    6. Discussion
    7. Technical details
  3. RESULTS
    1. Molecular C6 coefficients
    2. Noncovalent interactions and conformational energies
    3. Noncovalently bound complexes of molecules with heavier elements
    4. Binding energy between graphene sheets and in large aromatic complexes
    5. Thermochemistry
    6. Metallic systems
  4. SUMMARY AND CONCLUSION

RELATED DATABASES

To view database links for this article, you need to log in.

KEYWORDS and PACS

Keywords

ab initio calculations, adsorption, density functional theory, graphene, organic compounds, recursion method, silver

PACS

  • 31.15.em

    Corrections for core-spin polarization, surface effects, etc.

  • 31.15.aj

    Relativistic corrections, spin-orbit effects, fine structure; hyperfine structure

  • 68.43.Mn

    Adsorption kinetics

  • 68.43.Bc

    Ab initio calculations of adsorbate structure and reactions

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.3382344

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

For access to fully linked references, you need to log in.
    J. Gräfenstein and D. Cremer, J. Chem. Phys. 130, 124105 (2009)JCPSA6000130000012124105000001.

    T. Sato and H. Nakai, J. Chem. Phys. 131, 224104 (2009)JCPSA6000131000022224104000001.

    M. Elstner, P. Hobza, T. Frauenheim, S. Suhai, and E. Kaxiras, J. Chem. Phys. 114, 5149 (2001)JCPSA6000114000012005149000001.

    Y. Andersson, D. C. Langreth, and B. I. Lundqvist, Phys. Rev. Lett. 76, 102 (1996).

    O. A. von Lilienfeld, I. Tavernelli, U. Röthlisberger, and D. Sebastiani, Phys. Rev. Lett. 93, 153004 (2004).

    Y. Y. Sun, Y. -H. Kim, K. Lee, and S. B. Zhang, J. Chem. Phys. 129, 154102 (2008)JCPSA6000129000015154102000001.

    F. Shimojo, Z. Wu, A. Nakano, R. K. Kalia, and P. Vashishta, J. Chem. Phys. 132, 094106 (2010)JCPSA6000132000009094106000001.

    O. A. Vydrov and T. Van Voorhis, Phys. Rev. Lett. 103, 063004 (2009).

    K. Pernal, R. Podeszwa, K. Patkowski, and K. Szalewicz, Phys. Rev. Lett. 103, 263201 (2009).

    A. D. Becke, Phys. Rev. A 38, 3098 (1988).

    C. Lee, W. Yang, and R. G. Parr, Phys. Rev. B 37, 785 (1988).

    J. P. Perdew, Phys. Rev. B 33, 8822 (1986).

    J. P. Perdew, Phys. Rev. B 34, 7406 (1986).

    J. P. Perdew, K. Burke, and M. Ernzerhof, Phys. Rev. Lett. 77, 3865 (1996).

    Y. Zhang and W. Yang, Phys. Rev. Lett. 80, 890 (1998).

    J. Tao, J. P. Perdew, V. N. Staroverov, and G. E. Scuseria, Phys. Rev. Lett. 91, 146401 (2003).

    A. D. Becke, J. Chem. Phys. 98, 5648 (1993)JCPSA6000098000007005648000001.

    C. Adamo and V. Barone, J. Chem. Phys. 110, 6158 (1999)JCPSA6000110000013006158000001.

    S. Grimme, J. Chem. Phys. 124, 034108 (2006)JCPSA6000124000003034108000001.

    A. D. Becke and E. R. Johnson, J. Chem. Phys. 122, 154104 (2005)JCPSA6000122000015154104000001.

    A. D. Becke and E. R. Johnson, J. Chem. Phys. 123, 154101 (2005)JCPSA6000123000015154101000001.

    A. Tkatchenko and M. Scheffler, Phys. Rev. Lett. 102, 073005 (2009).

    A. D. Becke and E. R. Johnson, J. Chem. Phys. 124, 014104 (2006)JCPSA6000124000001014104000001.

    E. R. Johnson and A. D. Becke, J. Chem. Phys. 124, 174104 (2006)JCPSA6000124000017174104000001.

    E. R. Johnson and A. D. Becke, J. Chem. Phys. 123, 024101 (2005)JCPSA6000123000002024101000001.

    J. Kong, Z. Gan, E. Proynov, M. Freindorf, and T. R. Furlani, Phys. Rev. A 79, 042510 (2009).

    F. A. Gianturco and F. Paesani, J. Chem. Phys. 113, 3011 (2000)JCPSA6000113000008003011000001.

    X. Wu, M. C. Vargas, S. Nayak, V. Lotrich, and G. Scoles, J. Chem. Phys. 115, 8748 (2001)JCPSA6000115000019008748000001.

    Q. Wu and W. Yang, J. Chem. Phys. 116, 515 (2002)JCPSA6000116000002000515000001.

    U. Zimmerli, M. Parrinello, and P. Koumoutsakos, J. Chem. Phys. 120, 2693 (2004)JCPSA6000120000006002693000001.

    C. Kamal, T. K. Ghanty, A. Banerjee, and A. Chakrabarti, J. Chem. Phys. 131, 164708 (2009)JCPSA6000131000016164708000001.

    G. Starkschall and R. Gordon, J. Chem. Phys. 56, 2801 (1972)JCPSA6000056000006002801000001.

    A. Thakkar, H. Hettema, and P. Wormer, J. Chem. Phys. 97, 3252 (1992)JCPSA6000097000005003252000001.

    K. T. Tang and J. P. Toennies, J. Chem. Phys. 80, 3726 (1984)JCPSA6000080000008003726000001.

    N. A. deLima, J. Chem. Phys. 132, 014110 (2010)JCPSA6000132000001014110000001.

    A. Kumar and A. J. Thakkar, J. Chem. Phys. 132, 074301 (2010)JCPSA6000132000007074301000001.

    B. M. Axilrod and E. Teller, J. Chem. Phys. 11, 299 (1943)JCPSA6000011000006000299000001.

    A. Tkatchenko and O. A. von Lilienfeld, Phys. Rev. B 78, 045116 (2008).

    J. F. Dobson, A. White, and A. Rubio, Phys. Rev. Lett. 96, 073201 (2006).

    F. Weigend, F. Furche, and R. Ahlrichs, J. Chem. Phys. 119, 12753 (2003)JCPSA6000119000024012753000001.

    A. Schäfer, C. Huber, and R. Ahlrichs, J. Chem. Phys. 100, 5829 (1994)JCPSA6000100000008005829000001.

    B. Metz, H. Stoll, and M. Dolg, J. Chem. Phys. 113, 2563 (2000)JCPSA6000113000007002563000001.

    K. A. Peterson, D. Figgen, E. Goll, H. Stoll, and M. Dolg, J. Chem. Phys. 119, 11113 (2003)JCPSA6000119000021011113000001.

    S. Tsuzuki, K. Honda, T. Uchimaru, and M. Mikami, J. Chem. Phys. 124, 114304 (2006)JCPSA6000124000011114304000001.

    J. -D. Chai and M. Head-Gordon, J. Chem. Phys. 131, 174105 (2009)JCPSA6000131000017174105000001.

    A. Gulans, M. J. Puska, and R. M. Nieminen, Phys. Rev. B 79, 201105(R) (2009).

    R. Zacharia, H. Ulbricht, and T. Hertel, Phys. Rev. B 69, 155406 (2004).

    E. Ziambaras, J. Kleis, E. Schröder, and P. Hyldgaard, Phys. Rev. B 76, 155425 (2007).

    A. G. Donchev, Phys. Rev. B 74, 235401 (2006).

    E. R. Johnson, P. Mori-Sánchez, A. J. Cohen, and W. Yang, J. Chem. Phys. 129, 204112 (2008)JCPSA6000129000020204112000001.


For access to citing articles, you need to log in.


Figures (14) Tables (8)

Access to article objects (figures, tables, multimedia) requires a subscription; log in to view available files.
(Access to supplementary files, where available, is free for this journal.)

Access to article objects (figures, tables, multimedia) requires a subscription; log in to view available files.
(Access to supplementary files, where available, is free for this journal.)


Close

Google Calendar

ADVERTISEMENT

Your Recent History Recent History Help

Recently Viewed

  1. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
  2. Active-space completely-renormalized equation-of-motion coupled-cluster formalism: Excited-state studies of green fluorescent protein, free-base porphyrin, and oligoporphyrin dimer
  3. Electrolytes in porous electrodes: Effects of the pore size and the dielectric constant of the medium
  4. A theoretical study of H2 dissociation on (×)R30°CO/Ru(0001)
Go to AIP Home
Copyright © American Institute of Physics
close