Theoretical Study of Electron Transfer and Electron Transport Processes in Molecular Systems at Metal Substrates

  • Óscar Rubio-Pons
  • Rainer Härtle
  • Jingrui Li
  • Michael Thoss
Conference paper

Abstract

In this paper we present a study of electron transfer and electron transport processes in molecular systems at metal substrates. In particular, photoinduced electron transfer in molecules at metal surfaces and voltage driven electron transport in single-molecule junctions are investigated. The methodology is based on a combination of first-principle electronic structure methods to characterize the systems and dynamical basis-set as well as nonequilibrium Green’s function methods to study electron transfer dynamics and transport properties, respectively. The results show the ultrafast character of electron transfer at molecule-metal interfaces and demonstrate the importance of electronic-vibrational coupling in single-molecule junctions. Furthermore, a mechanism for photoinduced switching of molecular junctions based on hydrogen translocation is discussed.

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References

  1. 1.
    Vienna ab-intio simulation package (vasp), version 4.6/ http://cms.mpi.univie.ac.at/cmspage/main/ (2006)
  2. 2.
    Arnim, M.V., Ahlrichs, R.: J. Comput. Chem. 19, 1746 (1998) CrossRefGoogle Scholar
  3. 3.
    Barbara, P.F., Meyer, T.J., Ratner, M.A.: J. Phys. Chem. 100, 13148 (1996) CrossRefGoogle Scholar
  4. 4.
    Becke, A.D.: 98, 5648 (1993) Google Scholar
  5. 5.
    Benesch, C., Cizek, M., Klimes, J., Kondov, I., Thoss, M., Domcke, W.: J. Phys. Chem. C 112, 9880 (2008) CrossRefGoogle Scholar
  6. 6.
    Benesch, C., Rode, M., Cizek, M., Hartle, R., Rubio-Pons, O., Thoss, M., Sobolewski, A.: J. Phys. Chem. C 113, 10315 (2009) CrossRefGoogle Scholar
  7. 7.
    Boroda, Y.G., Calhoun, A., Voth, G.A.: J. Chem. Phys. 107, 8940 (1997) CrossRefGoogle Scholar
  8. 8.
    Choi, B.Y., Kahng, S.J., Kim, S., Kim, H., Kim, H., Song, Y., Ihm, J., Kuk, Y.: Phys. Rev. Lett. 96, 156106 (2006) CrossRefGoogle Scholar
  9. 9.
    Cuniberti, G., Fagas, G., Richter, K.: Introducing Molecular Electronics. Springer, Heidelberg (2005) CrossRefGoogle Scholar
  10. 10.
    Dulic, D., van der Molen, S., Kudernac, T., Jonkman, H., de Jong, J., Bowden, T., van Esch, J., Feringa, B., van Wees, B.: Phys. Rev. Lett. 91, 207402 (2003) CrossRefGoogle Scholar
  11. 11.
    Ernstorfer, R., Gundlach, L., Felber, S., Storck, W., Eichberger, R., Willig, F.: J. Phys. Chem. B 110, 25383 (2006) CrossRefGoogle Scholar
  12. 12.
    Fölisch, A., Feulner, P., Fink, A., Menzel, D., Sanchez-Portal, D., Echenique, P., W. Wurth: Nature (London) 436, 373 (2005) CrossRefGoogle Scholar
  13. 13.
  14. 14.
    Frey, S., Shaporenko, A., Zharnikov, M., Harder, P., Allara, D.L.: J. Phys. Chem. B 107, 7716 (2005) CrossRefGoogle Scholar
  15. 15.
    Galperin, M., Ratner, M., Nitzan, A.: Phys. Rev. B 73, 045314 (2006) CrossRefGoogle Scholar
  16. 16.
    Galperin, M., Ratner, M.A., Nitzan, A.: Molecular transport junctions: vibrational effects. J. Phys.: Condens. Matter 19, 103201 (2007) CrossRefGoogle Scholar
  17. 17.
    Grätzel, M.: Nature 414, 338 (2001) CrossRefGoogle Scholar
  18. 18.
    Hagfeldt, A., Grätzel, M.: Chem. Rev. 95, 49 (1995) CrossRefGoogle Scholar
  19. 19.
    Härtle, R., Benesch, C., Thoss, M.: Multimode vibrational effects in single-molecule conductance: A nonequilibrium green’s function approach. Phys. Rev. B 77, 205314 (2008) CrossRefGoogle Scholar
  20. 20.
    Härtle, R., Benesch, C., Thoss, M.: Phys. Rev. Lett. 102, 146801 (2009) CrossRefGoogle Scholar
  21. 21.
    Härtle, R., Benesch, C., Thoss, M.: Vibrational nonequilibrium effects in the conductance of single molecules with multiple electronic states. Phys. Rev. Lett. 102, 146801 (2009) CrossRefGoogle Scholar
  22. 22.
  23. 23.
    Huber, R., Moser, J.E., Grätzel, M., Wachtveitl, J.: Chem. Phys. Lett. 285, 39 (2002) Google Scholar
  24. 24.
    Jortner, J., Bixon, M.: Electron Transfer: From Isolated Molecules to Biomolecules, Dynamics and Spectroscopy Adv. Chem. Phys. Vols. 106-107. Wiley, New York (1999) Google Scholar
  25. 25.
    Kondov, I., Cizek, M., Benesch, C., Wang, H., Thoss, M.: J. Phys. Chem. C 111, 11970 (2007) CrossRefGoogle Scholar
  26. 26.
    Kresse, G., Joubert, J.: Phys. Rev. B 59, 1758 Google Scholar
  27. 27.
    Li, J., Speyer, G., Sankey, O.: Phys. Rev. Lett. 93, 248302 (2004) CrossRefGoogle Scholar
  28. 28.
    M. del Valle, Gutierrez, R., Tejedor, C., Cuniberti, G.: Nature Nanotech. 2, 176 (2007) CrossRefGoogle Scholar
  29. 29.
    Michel-Beyerle, M.E.: The Reaction Center of Photosynthetic Bacteria: Structure and Dynamics. Springer, Berlin (1996) Google Scholar
  30. 30.
    Ragan, S., Gallet, J.J., Bournel, F., Kubsky, S., Guen, K.L., Dugour, G., Rochet, F., Sirotti, F., Carninato, S., Ilakovac, V.: Phys. Rev. B 71, 165318 (2005) CrossRefGoogle Scholar
  31. 31.
    Rubio-Pons, O., Hartle, R., Thoss, M.: HLRBII project (pr28lo) (2009) Google Scholar
  32. 32.
    Schnadt, J., Brühwiler, P.A., Patthey, L., O’Shea, J.N., Södergreen, S., Odellus, M., Ahuja, R., Karis, O., Bässler, M., Persson, P., Siegbahn, H., Lunell, S., Martenson, N.: Nature 418, 620 (2002) CrossRefGoogle Scholar
  33. 33.
    Shemesh, D., Domcke, W.: HLRBII project (h0833) (2008) Google Scholar
  34. 34.
    Sobolewski, A.: Phys. Chem. Chem. Phys. 10, 1243 (2008) CrossRefGoogle Scholar
  35. 35.
    Sobolewski, A., Domcke, W., Hättig, C.: J. Phys. Chem. A 110, 6301 (2006) CrossRefGoogle Scholar
  36. 36.
    Tominaga, K., Kliner, D.A.V., Johnson, A.E., Levinger, N.E., Barbara, P.F.: J. Chem. Phys. 98, 1228 (1993) CrossRefGoogle Scholar
  37. 37.
    Wang, C., Mohney, B.K., Williams, R.D., Petrov, V., Hupp, J.T., Walker, G.C.: J. Am. Chem. Soc. 120, 5848 (1998) CrossRefGoogle Scholar
  38. 38.
    Xue, Y., Ratner, M.: Phys. Rev. B 68, 115406 (2001) CrossRefGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2010

Authors and Affiliations

  • Óscar Rubio-Pons
    • 1
  • Rainer Härtle
    • 2
  • Jingrui Li
    • 1
  • Michael Thoss
    • 2
  1. 1.Lehrstuhl für Theoretische ChemieTechnische Universität MünchenGarchingGermany
  2. 2.Institut für Theoretische PhysikUniversität Erlangen-NürnbergErlangenGermany

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