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Theory of action spectroscopy for single-molecule reactions induced by vibrational excitations with STM
Donostia Int Phys Ctr DIPC UPV EHU, San Sebastian 20018, Spain.
Linnaeus University, Faculty of Technology, Department of Physics and Electrical Engineering. Toyama Univ, Grad Sch Sci & Engn, Div Nano & New Funct Mat Sci, Toyama 930855, Japan.
Toyama Univ, Grad Sch Sci & Engn, Div Nano & New Funct Mat Sci, Toyama 930855, Japan.
2014 (English)In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 89, no 3, p. 035427-Article in journal (Refereed) Published
Abstract [en]

A theory of action spectroscopy, i.e., a reaction rate or yield as a function of bias voltage, is presented for single-molecule reactions induced by the inelastic tunneling current with a scanning tunneling microscope. A formula for the reaction yield is derived using the adsorbate resonance model, which provides a versatile tool to analyze vibrationally mediated reactions of single adsorbates on conductive surfaces. This allows us to determine the energy quantum of the excited vibrational mode, the effective broadening of the vibrational density of states (as described by Gaussian or Lorentzian functions), and a prefactor characterizing the elementary process behind the reaction. The underlying approximations are critically discussed. We point out that observation of reaction yields at both bias voltage polarities can provide additional insight into the adsorbate density of states near the Fermi level. As an example, we apply the theory to the case of flip motion of a hydroxyl dimer (OD)(2) on Cu(110) which was experimentally observed by Kumagai et al. [Phys. Rev. B 79, 035423 (2009)]. In combination with density functional theory calculations for the vibrational modes, the vibrational damping due to electron-hole pair generation, and the potential energy landscape for the flip motion, a detailed microscopic picture for the switching process is established. This picture reveals that the predominant mechanism is excitation of the OD stretch modes which couple anharmonically to the low-energy frustrated rotation mode.

Place, publisher, year, edition, pages
2014. Vol. 89, no 3, p. 035427-
National Category
Physical Sciences
Research subject
Natural Science, Physics
Identifiers
URN: urn:nbn:se:lnu:diva-33350DOI: 10.1103/PhysRevB.89.035427ISI: 000332232300004Scopus ID: 2-s2.0-84893139363OAI: oai:DiVA.org:lnu-33350DiVA, id: diva2:708240
Available from: 2014-03-27 Created: 2014-03-27 Last updated: 2017-12-05Bibliographically approved

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Paulsson, Magnus

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