{
  "id": "1106.0170",
  "version": "v1",
  "published": "2011-06-01T13:19:16.000Z",
  "updated": "2011-06-01T13:19:16.000Z",
  "title": "Bias-Controlled Selective Excitation of Vibrational Modes in Molecular Junctions: A Route Towards Mode-Selective Chemistry",
  "authors": [
    "R. Volkovich",
    "R. Härtle",
    "M. Thoss",
    "U. Peskin"
  ],
  "comment": "46 pages, 17 figures, accepted in PCCP",
  "journal": "Phys. Chem. Chem. Phys. 13, 14333 (2011)",
  "doi": "10.1039/C1CP21161G",
  "categories": [
    "cond-mat.mes-hall"
  ],
  "abstract": "We show that individual vibrational modes in single-molecule junctions with asymmetric molecule-lead coupling can be selectively excited by applying an external bias voltage. Thereby, a non-statistical distribution of vibrational energy can be generated, that is, a mode with a high frequency can be stronger excited than a mode with a lower frequency. This is of particular interest in the context of mode-selective chemistry, where one aims to break specific (not necessarily the weakest) chemical bond in a molecule. Such mode-selective vibrational excitation is demonstrated for two generic model systems representing asymmetric molecular junctions and/or scanning tunneling microscopy experiments. To this end, we employ two complementary theoretical approaches, a nonequilibrium Green's function approach and a master equation approach. The comparison of both methods reveals good agreement in describing resonant electron transport through a single-molecule contact, but also highlights the role of non-resonant transport processes, in particular co-tunneling and off-resonant electron-hole pair creation processes.",
  "revisions": [
    {
      "version": "v1",
      "updated": "2011-06-01T13:19:16.000Z"
    }
  ],
  "analyses": {
    "keywords": [
      "vibrational modes",
      "bias-controlled selective excitation",
      "mode-selective chemistry",
      "systems representing asymmetric molecular",
      "model systems representing asymmetric"
    ],
    "tags": [
      "journal article"
    ],
    "publication": {
      "journal": "Physical Chemistry Chemical Physics (Incorporating Faraday Transactions)",
      "year": 2011,
      "volume": 13,
      "number": 32,
      "pages": 14333
    },
    "note": {
      "typesetting": "TeX",
      "pages": 46,
      "language": "en",
      "license": "arXiv",
      "status": "editable",
      "adsabs": "2011PCCP...1314333V"
    }
  }
}