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Phys. Rev. Lett. 86, 1566–1569 (2001)

Novel Surface Vibrational Spectroscopy: Infrared-Infrared-Visible Sum-Frequency Generation

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Mischa Bonn*
Leiden Institute of Chemistry, P.O. Box 9502, 2300 RA Leiden, The Netherlands
and Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany

Christian Hess and James H. Miners
Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany

Tony F. Heinz
Department of Physics, Columbia University, 538 West 120th Street, New York, New York 10027

Huib J. Bakker
FOM–Institute for Atomic and Molecular Physics, Kruislaan 407, 1098 SJ Amsterdam, The Netherlands

Minhaeng Cho
Department of Chemistry and Center for Multidimensional Spectroscopy, Korea University, Seoul 136-701, Korea

Received 5 October 2000; published in the issue dated 19 February 2001

A novel type of surface vibrational sum-frequency generation spectroscopy is presented that enables a highly specific measurement of the coupling of molecules on surfaces. With this doubly vibrationally resonant technique, two-dimensional vibrational spectroscopy of molecules on surfaces becomes possible. The technique is demonstrated for the C-O stretch vibration of CO on a ruthenium (001) surface. It allows for the determination of the intermolecular coupling strength of dipole-coupled CO molecules on the surface.

© 2001 The American Physical Society

URL:
http://link.aps.org/doi/10.1103/PhysRevLett.86.1566
DOI:
10.1103/PhysRevLett.86.1566
PACS:
68.35.Ja, 33.20.Ea, 33.40.+f, 42.65.-k

*Email address: m.bonn@chem.leidenuniv.nl