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Journal of Chemical Physics / Volume 98 / Issue 12

J. Chem. Phys. 98, 9986 (1993); http://dx.doi.org/10.1063/1.464324 (9 pages)

Picosecond measurement of substrate‐to‐adsorbate energy transfer: The frustrated translation of CO/Pt(111)

T. A. Germer, J. C. Stephenson, E. J. Heilweil, and R. R. Cavanagh

National Institute of Standards and Technology, Gaithersburg, Maryland 20899

(Received 28 December 1992; accepted 12 March 1993)

The transient infrared response of CO/Pt(111) following picosecond visible excitation is reported. A spectrally broad decrease in reflectivity correlates with heating of the Pt lattice, and an observed shift in the CO(v=0→1) transition is interpreted as heating of the 60 cm−1 in‐plane frustrated translational mode. A phenomenological three temperature model that assumes the adsorbate vibrational temperature Tads exclusively couples to either the electronic temperature Te (with a time constant τe) or to the lattice temperature Tlat (with a time constant τlat) describes the temporal response of the adsorbate vibrations. The lattice phonon temperature Tlat(z,t) and measured temperature dependence of the optical constants predict the observed spectrally broad reflectivity change. Density matrix methods model the infrared response of the transiently heated molecule. Limits of τe=2±1 ps or τlat<1 ps are established by comparison of predicted spectra and the data.

KEYWORDS and PACS

Keywords

PS RANGE, ENERGY TRANSFER, ADSORBATES, SUBSTRATES, FRUSTRATION, DISPLACEMENTS, CARBON MONOXIDE, PLATINUM, INFRARED SPECTRA, EXCITATION, VISIBLE RADIATION, REFLECTIVITY, ELECTRON TEMPERATURE, TEMPERATURE DEPENDENCE, OPTICAL PROPERTIES, DENSITY MATRIX, HEATING

PACS

  • 82.20.Rp

    State to state energy transfer

  • 82.65.+r

    Surface and interface chemistry; heterogeneous catalysis at surfaces

  • 78.47.-p

    Spectroscopy of solid state dynamics

  • 78.20.Ci

    Optical constants (including refractive index, complex dielectric constant, absorption, reflection and transmission coefficients, emissivity)

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.464324

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

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