Letter abstract


Nature Materials 7, 38 - 42 (2008)
Published online: 25 November 2007 | doi:10.1038/nmat2066

Subject Categories: Molecular electronics | Nanoscale materials | Computation, modelling and theory

Spatially resolved electronic and vibronic properties of single diamondoid molecules

Yayu Wang1, Emmanouil Kioupakis1, Xinghua Lu1, Daniel Wegner1, Ryan Yamachika1, Jeremy E. Dahl2, Robert M. K. Carlson2, Steven G. Louie1 & Michael F. Crommie1

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Diamondoids are a unique form of carbon nanostructure best described as hydrogen-terminated diamond molecules1. Their diamond-cage structures and tetrahedral sp3 hybrid bonding create new possibilities for tuning electronic bandgaps, optical properties, thermal transport and mechanical strength at the nanoscale1, 2. The recently discovered higher diamondoids3, 4 have thus generated much excitement in regards to their potential versatility as nanoscale devices5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15. Despite this excitement, however, very little is known about the properties of isolated diamondoids on metal surfaces, a very relevant system for molecular electronics. For example, it is unclear how the microscopic characteristics of molecular orbitals and local electron–vibrational coupling affect electron conduction, emission and energy transfer in the diamondoids. Here, we report the first single-molecule study of tetramantane diamondoids on Au(111) using scanning tunnelling microscopy and spectroscopy. We find that the diamondoid electronic structure and electron–vibrational coupling exhibit unique and unexpected spatial correlations characterized by pronounced nodal structure across the molecular surfaces. Ab initio pseudopotential density functional calculations reveal that much of the observed electronic and vibronic properties of diamondoids are determined by surface hydrogen terminations, a feature having important implications for designing future diamondoid-based molecular devices.

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  1. Department of Physics, University of California at Berkeley, and Materials Sciences Division, Lawrence Berkeley Laboratory, Berkeley, California 94720-7300, USA
  2. MolecularDiamond Technology, Chevron Technology Ventures, Richmond, California 94802, USA

Correspondence to: Yayu Wang1 e-mail: yywang@berkeley.edu

Correspondence to: Michael F. Crommie1 e-mail: crommie@berkeley.edu



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