title: Single-Molecule Dynamics in the Presence of Strong Intermolecular Interactions.
abstract: In contrast to conventional spectroscopic studies of adsorbates at high coverage that provide only spatially averaged information, we have characterized the laterally confined shuttling dynamics of a single molecule under the influence of intermolecular interactions by vibrational spectroscopy using a scanning tunneling microscope. The bridge sites on Pt(111) are only occupied by a CO molecule that is surrounded by four other CO molecules at on-top sites. The bridge-site CO undergoes laterally confined shuttling toward an adjacent on-top site to transiently occupy a metastable site, which is slightly displaced from the center of an on-top site through repulsive interaction with adjacent on-top CO molecules. Analysis of action spectra for the shuttling events reveals the C-O stretch frequency of the metastable CO. We also constructed a modified potential energy surface incorporating the intermolecular interaction, which reveals the underlying mechanism and provides a new way to experimentally determine detailed information on the energetics of the metastable state.
authors: Department of Advanced Materials Science, The University of Tokyo , 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8561, Japan.|Surface and Interface Science Laboratory, RIKEN , 2-1 Hirosawa, Wako, Saitama 351-0198, Japan.
authors: Hyun Jin
authors: HJ
authors: Yang
authors: Department of Chemistry, University of Illinois at Chicago , 845 West Taylor Street, Chicago, Illinois 60607, United States.
authors: Michael
authors: M
authors: Trenary
authors: Department of Advanced Materials Science, The University of Tokyo , 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8561, Japan.
authors: Maki
authors: M
authors: Kawai
authors: Surface and Interface Science Laboratory, RIKEN , 2-1 Hirosawa, Wako, Saitama 351-0198, Japan.
authors: Yousoo
authors: Y
authors: Kim