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Nonlinear optical response of a gold surface in the visible range: A study by two-color sum-frequency generation spectroscopy. III. Simulations of the experimental SFG intensities
Univ Paris Saclay, Univ Paris Sud, Lab Chim Phys, CNRS, Batiment 201 P2, F-91405 Orsay, France..
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry. Univ Paris Saclay, Univ Paris Sud, Lab Chim Phys, CNRS, Batiment 201 P2, F-91405 Orsay, France.;KTH Royal Inst Technol, Dept Chem, Sch Chem Sci & Engn, SE-10044 Stockholm, Sweden.;Acad Sinica, Inst Phys, Taipei 11529, Taiwan..
2018 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 149, no 15, article id 154701Article in journal (Refereed) Published
Abstract [en]

We model the amplitude line shape and absolute phase of the infrared-visible sum-frequency signals produced by a thiolated polycrystalline gold surface as a function of the visible wavelength. We follow two hypotheses: in the interband scenario, the resonant features are attributed to interband transitions, whereas in the effective surface state scenario, they stem mostly from the excitation of surface transitions. We find that both scenarios lead to a satisfactory account of the experimental data and that only free electrons may spill out of the gold bulk, as expected. For the interband scenario, the balance between free and bound electron contributions to sum-frequency generation has to be adjusted to fit the data. The surface transitions are shown to take their origin inside gold and we investigate the surface states involved in such transitions, with a comparison to the silver surfaces. We finally provide a work program dedicated to discriminate between the two scenarios. Published by AIP Publishing.

Place, publisher, year, edition, pages
AMER INST PHYSICS , 2018. Vol. 149, no 15, article id 154701
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Physical Sciences
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URN: urn:nbn:se:kth:diva-239098DOI: 10.1063/1.5047098ISI: 000448216600028PubMedID: 30342449Scopus ID: 2-s2.0-85054990950OAI: oai:DiVA.org:kth-239098DiVA, id: diva2:1264836
Note

QC 20181121

Available from: 2018-11-21 Created: 2018-11-21 Last updated: 2018-11-21Bibliographically approved

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