Non-linear optical studies of adsorbates: Spectroscopy and dynamics

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In the first part of this thesis, we have established a systematic procedure to apply the surface optical second-harmonic generation (SHG) technique to study surface dynamics of adsorbates. In particular, we have developed a novel technique for studies of molecular surface diffusions. In this technique, the laser-induced desorption with two interfering laser beams is used to produce a monolayer grating of adsorbates. The monolayer grating is detected with diffractions of optical SHG. By monitoring the first-order second-harmonic diffraction, we can follow the time evolution of the grating modulation from which we are able to deduce the diffusion constant of the ... continued below

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Pages: (178 p)

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Zhu, Xiangdong. August 1, 1989.

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Description

In the first part of this thesis, we have established a systematic procedure to apply the surface optical second-harmonic generation (SHG) technique to study surface dynamics of adsorbates. In particular, we have developed a novel technique for studies of molecular surface diffusions. In this technique, the laser-induced desorption with two interfering laser beams is used to produce a monolayer grating of adsorbates. The monolayer grating is detected with diffractions of optical SHG. By monitoring the first-order second-harmonic diffraction, we can follow the time evolution of the grating modulation from which we are able to deduce the diffusion constant of the adsorbates on the surface. We have successfully applied this technique to investigate the surface diffusion of CO on Ni(111). The unique advantages of this novel technique will enable us to readily study anisotropy of a surface diffusion with variable grating orientation, and to investigate diffusion processes of a large dynamic range with variable grating spacings. In the second part of this work, we demonstrate that optical infrared-visible sum-frequency generation (SFG) from surfaces can be used as a viable surface vibrational spectroscopic technique. We have successfully recorded the first vibrational spectrum of a monolayer of adsorbates using optical infrared-visible SFG. The qualitative and quantitative correlation of optical SFG with infrared absorption and Raman scattering spectroscopies are examined and experimentally demonstrated. We have further investigated the possibility to use transient infrared-visible SFG to probe vibrational transients and ultrafast relaxations on surfaces. 146 refs.

Physical Description

Pages: (178 p)

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NTIS, PC A09/MF A01; OSTI; INIS; GPO Dep.

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  • Other Information: Thesis (Ph.D.)

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  • Other: DE90001543
  • Report No.: LBL-27694
  • Grant Number: AC03-76SF00098
  • DOI: 10.2172/5538721 | External Link
  • Office of Scientific & Technical Information Report Number: 5538721
  • Archival Resource Key: ark:/67531/metadc1093631

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Reports, articles and other documents harvested from the Office of Scientific and Technical Information.

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  • August 1, 1989

Added to The UNT Digital Library

  • Feb. 10, 2018, 10:06 p.m.

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  • April 26, 2018, 11:52 a.m.

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Zhu, Xiangdong. Non-linear optical studies of adsorbates: Spectroscopy and dynamics, report, August 1, 1989; [Berkeley,] California. (digital.library.unt.edu/ark:/67531/metadc1093631/: accessed November 17, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.