• 文献标题:   Ultrafast Bidirectional Charge Transport and Electron Decoherence at Molecule/Surface Interfaces: A Comparison of Gold, Graphene, and Graphene Nanoribbon Surfaces
  • 文献类型:   Article
  • 作  者:   ADAK O, KLADNIK G, BAVDEK G, COSSARO A, MORGANTE A, CVETKO D, VENKATARAMAN L
  • 作者关键词:   charge transfer dynamic, photoemission spectroscopy, corehole clock, moleculemetal interface, moleculegraphene interface, charge decoherence
  • 出版物名称:   NANO LETTERS
  • ISSN:   1530-6984 EI 1530-6992
  • 通讯作者地址:   Univ Ljubljana
  • 被引频次:   12
  • DOI:   10.1021/acs.nanolett.5b03962
  • 出版年:   2015

▎ 摘  要

We investigate bidirectional femtosecond charge transfer dynamics using the core-hole clock implementation of resonant photoemission spectroscopy from 4,4'-bipyridine molecular layers on three different surfaces: Au(111), epitaxial graphene on Ni(111), and graphene nanoribbons. We show that the lowest unoccupied molecular orbital (LUMO) of the molecule drops partially below the Fermi level upon core-hole creation in all systems, opening an additional decay channel for the core-hole, involving electron donation from substrate to the molecule. Furthermore, using the core-hole clock method, we find that the bidirectional charge transfer time between the substrate and the molecule is fastest on Au(111), with a 2 fs time, then around 4 fs for epitaxial graphene and slowest with graphene nanoribbon surface, taking around 10 fs. Finally, we provide evidence for fast phase decoherence of the core-excited LUMO* electron through an interaction with the substrate providing the first observation of such a fast bidirectional charge transfer across an organic/graphene interface.