Quantitative molecular orbital energies within a G0W0 approximation

  • S. Sharifzadeh
  • I. Tamblyn
  • P. Doak
  • P. T. Darancet
  • J. B. Neaton
Regular Article
Part of the following topical collections:
  1. Topical issue: Challenges and solutions in GW calculations for complex systems

Abstract

Using many-body perturbation theory within a G0W0 approximation, with a plane wave basis set and using a starting point based on density functional theory within the generalized gradient approximation, we explore routes for computing the ionization potential (IP), electron affinity (EA), and fundamental gap of three gas-phase molecules — benzene, thiophene, and (1,4) diamino-benzene — and compare with experiments. We examine the dependence of the IP and fundamental gap on the number of unoccupied states used to represent the dielectric function and the self energy, as well as the dielectric function plane-wave cutoff. We find that with an effective completion strategy for approximating the unoccupied subspace, and a well converged dielectric function kinetic energy cutoff, the computed IPs and EAs are in excellent quantitative agreement with available experiment (within 0.2 eV), indicating that a one-shot G0W0 approach can be very accurate for calculating addition/removal energies of small organic molecules.

Keywords

Topical issue: Challenges and solutions in GW calculations for complex systems. Guest editors: Feliciano Giustino, Paolo Umari and Angel Rubio 

References

  1. 1.
    M. Scharber, D. Mühlbacher, M. Koppe, P. Denk, C. Waldauf, A. Heeger, C. Brabec, Adv. Mater. 18, 789 (2006)CrossRefGoogle Scholar
  2. 2.
    M.T. Lloyd, J.E. Anthony, G.G. Malliaras, Mater. Today 10, 34 (2007)CrossRefGoogle Scholar
  3. 3.
    B. Kippelen, J.L. Bredas, Energy Environ. Sci. 2, 251 (2009)CrossRefGoogle Scholar
  4. 4.
    A.J. Bard, Science 207, 139 (1980) ADSCrossRefGoogle Scholar
  5. 5.
    Z.V. Vardeny, A.J. Heeger, A. Dodabalapur, Synt. Met. 148, 1 (2005)CrossRefGoogle Scholar
  6. 6.
    T. Körzdörfer, S. Kümmel, N. Marom, L. Kronik, Phys. Rev. B 79, 201205 (2009) ADSCrossRefGoogle Scholar
  7. 7.
    T. Körzdörfer, S. Kümmel, N. Marom, L. Kronik, Phys. Rev. B 82, 129903 (2010) ADSCrossRefGoogle Scholar
  8. 8.
    S. Kümmel, L. Kronik, Rev. Mod. Phys. 80, 3 (2008)ADSCrossRefGoogle Scholar
  9. 9.
    S. Sharifzadeh, A. Biller, L. Kronik, J.B. Neaton, Phys. Rev. B 85, 125307 (2012) ADSCrossRefGoogle Scholar
  10. 10.
    I. Tamblyn, P. Darancet, S.Y. Quek, S.A. Bonev, J.B. Neaton, Phys. Rev. B 84, 201402 (2011) ADSCrossRefGoogle Scholar
  11. 11.
    M.S. Hybertsen, S.G. Louie, Phys. Rev. B 34, 5390 (1986) ADSCrossRefGoogle Scholar
  12. 12.
    C. Faber, C. Attaccalite, V. Olevano, E. Runge, X. Blase, Phys. Rev. B 83, 115123 (2011) ADSCrossRefGoogle Scholar
  13. 13.
    X. Blase, C. Attaccalite, V. Olevano, Phys. Rev. B 83, 115103 (2011) ADSCrossRefGoogle Scholar
  14. 14.
    X. Blase, C. Attaccalite, Appl. Phys. Lett. 99, 171909 (2011) ADSCrossRefGoogle Scholar
  15. 15.
    C. Rostgaard, K.W. Jacobsen, K.S. Thygesen, Phys. Rev. B 81, 085103 (2010) ADSCrossRefGoogle Scholar
  16. 16.
    X. Qian, P. Umari, N. Marzari, Phys. Rev. B 84, 075103 (2011) ADSCrossRefGoogle Scholar
  17. 17.
    G. Samsonidze, M. Jain, J. Deslippe, M.L. Cohen, S.G. Louie, Phys. Rev. Lett. 107, 186404 (2011) ADSCrossRefGoogle Scholar
  18. 18.
    P. Umari, G. Stenuit, S. Baroni, Phys. Rev. B 79, 201104 (2009) ADSCrossRefGoogle Scholar
  19. 19.
    P. Umari, G. Stenuit, S. Baroni, Phys. Rev. B 81, 115104 (2010) ADSCrossRefGoogle Scholar
  20. 20.
    M. Strange, C. Rostgaard, H. Häkkinen, K.S. Thygesen, Phys. Rev. B 83, 115108 (2011) ADSCrossRefGoogle Scholar
  21. 21.
    X. Ren, P. Rinke, V. Blum, J. Wieferink, A. Tkatchenko, A. Sanfilippo, K. Reuter, M. Scheffler, New J. Phys. 14, 053020 (2012) ADSCrossRefGoogle Scholar
  22. 22.
    G. Onida, L. Reining, A. Rubio, Rev. Mod. Phys. 74, 601 (2002)ADSCrossRefGoogle Scholar
  23. 23.
    P. García-Gonzalez, R.W. Godby, Phys. Rev. Lett. 88, 056406 (2002) ADSCrossRefGoogle Scholar
  24. 24.
    P. García-Gonzlez, R.W. Godby, Phys. Rev. B 63, 075112 (2001) ADSCrossRefGoogle Scholar
  25. 25.
    W.G. Aulbur, L. Jönsson, J.W. Wilkins, in Solid State Physics, edited by H. Ehrenreich, F. Spaepen (Academic Press, 1999), Vol. 54, pp. 1–218Google Scholar
  26. 26.
    L. Kronik, R. Fromherz, E. Ko, G. Gantefor, J.R. Chelikowsky, Eur. Phys. J. D 24, 33 (2003)ADSCrossRefGoogle Scholar
  27. 27.
    S.G. Lias, in NIST Chemistry WebBook, NIST Standard Reference Database Number 69, edited by P. Linstrom, W. Mallartd (National Institute of Standards and Technology, Gaithersburg, MD, 2012), http://webbook.nist.gov
  28. 28.
    D.E. Cabelli, A.H. Cowley, M.J.S. Dewar, J. Am. Chem. Soc. 103, 3286 (1981) CrossRefGoogle Scholar
  29. 29.
    D. Streets, W. Elane Hall, G.P. Ceasar, Chem. Phys. Lett. 17, 90 (1972)ADSCrossRefGoogle Scholar
  30. 30.
    P.D. Burrow, J.A. Michejda, K.D. Jordan, J. Chem. Phys. 86, 9 (1987)ADSCrossRefGoogle Scholar
  31. 31.
    J. Deslippe, G. Samsonidze, D.A. Strubbe, M. Jain, M.L. Cohen, S.G. Louie, Comput. Phys. Commun. 183, 1269 (2012) ADSCrossRefGoogle Scholar
  32. 32.
    J.P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett. 77, 3865 (1996) ADSCrossRefGoogle Scholar
  33. 33.
    M.S. Hybertsen, S.G. Louie, Phys. Rev. B 35, 5585 (1987) ADSCrossRefGoogle Scholar
  34. 34.
    P.E. Trevisanutto, C. Giorgetti, L. Reining, M. Ladisa, V. Olevano, Phys. Rev. Lett. 101, 226405 (2008) ADSCrossRefGoogle Scholar
  35. 35.
    B. Shih, Y. Xue, P. Zhang, M.L. Cohen, S.G. Louie, Phys. Rev. Lett. 105, 146401 (2010) ADSCrossRefGoogle Scholar
  36. 36.
    L. Hedin, Phys. Rev. 139, A796 (1965) ADSCrossRefGoogle Scholar
  37. 37.
    F. Bruneval, X. Gonze, Phys. Rev. B 78, 085125 (2008) ADSCrossRefGoogle Scholar
  38. 38.
    J. Deslippe, M. Jain, G. Samsonidze, M.L. Cohen, S.G. Louie, to be submitted (2012)Google Scholar
  39. 39.
    W. Kang, M.S. Hybertsen, Phys. Rev. B 82, 195108 (2010) ADSCrossRefGoogle Scholar
  40. 40.
    F. Giustino, M.L. Cohen, S.G. Louie, Phys. Rev. B 81, 115105 (2010) ADSCrossRefGoogle Scholar
  41. 41.
    J.A. Berger, L. Reining, F. Sottile, Phys. Rev. B 82, 041103 (2010) ADSCrossRefGoogle Scholar
  42. 42.
    L. Reining, G. Onida, R.W. Godby, Phys. Rev. B 56, R4301 (1997) ADSCrossRefGoogle Scholar
  43. 43.
    W. Kang, M.S. Hybertsen, Phys. Rev. B 82, 085203 (2010) ADSCrossRefGoogle Scholar
  44. 44.
    E. Van Veen, Chem. Phys. Lett. 41, 535 (1976)ADSCrossRefGoogle Scholar

Copyright information

© EDP Sciences, SIF, Springer-Verlag Berlin Heidelberg 2012

Authors and Affiliations

  • S. Sharifzadeh
    • 1
  • I. Tamblyn
    • 1
    • 2
  • P. Doak
    • 1
    • 3
  • P. T. Darancet
    • 1
  • J. B. Neaton
    • 1
  1. 1.Molecular FoundryLawrence Berkeley National LaboratoryBerkeleyUSA
  2. 2.Physical and Life Sciences Directorate, Chemical Sciences DivisionLawrence Livermore National LaboratoryLivermoreUSA
  3. 3.Department of ChemistryUniversity of CaliforniaBerkeleyUSA

Personalised recommendations