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Journal of Chemical Physics / Volume 134 / Issue 8 / ARTICLES / Surfaces, Interfaces, and Materials

J. Chem. Phys. 134, 084701 (2011); http://dx.doi.org/10.1063/1.3518457 (7 pages)

Ultrafast vibrational dynamics and spectroscopy of a siloxane self-assembled monolayer

Satoshi Nihonyanagi, Ali Eftekhari-Bafrooei, and Eric Borguet

Department of Chemistry, Temple University, Philadelphia, Pennsylvania 19122, USA

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(Received 9 August 2010; accepted 1 November 2010; published online 22 February 2011)

Time and frequency domain sum-frequency generation (SFG) were combined to study the dynamics and structure of self-assembled monolayers (SAMs) on a fused silica surface. SFG-free induction decay (SFG-FID) of octadecylsilane SAM in the CH stretching region shows a relatively long time scale oscillation that reveals that six vibrational modes are involved in the response of the system. Five of the modes have commonly been used for the fitting of SFG spectra in the CH stretching region, namely the symmetric stretch and Fermi resonance of the methyl group, the antisymmetric stretch of the methyl, as well as the symmetric and antisymmetric stretches of the methylene group. The assignment of the sixth mode to the terminal CH2 group was confirmed by performing a density function theory calculation. The SFG-FID measures the vibrational dephasing time (T2) of each of the modes, including a specific CH2 group within the SAM, the terminal CH2, which had never been measured before. The relatively long (∼1.3 ps) dephasing of the terminal CH2 suggests that alkyl monolayer structure is close to that of the liquid condensed phase of Langmuir Blodgett films.

© 2011 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. EXPERIMENTAL
  3. RESULTS AND DISCUSSION
    1. Fitting
    2. Assignment of peaks
    3. Dephasing
  4. CONCLUSION

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KEYWORDS and PACS

Keywords

density functional theory, Fermi level, Fermi resonance, frequency-domain analysis, infrared spectra, monolayers, optical frequency conversion, organic compounds, self-assembly, time-domain analysis, vibrational modes, visible spectra

PACS

  • 81.05.Lg

    Polymers and plastics; rubber; synthetic and natural fibers; organometallic and organic materials

  • 78.30.Jw

    Organic compounds, polymers

  • 78.40.Me

    Organic compounds and polymers

  • 42.65.Ky

    Frequency conversion; harmonic generation, including higher-order harmonic generation

  • 73.20.At

    Surface states, band structure, electron density of states

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.3518457

PUBLICATION DATA

ISSN

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

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

For access to fully linked references, you need to log in.
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