Hofmann, Matthias J. and Koelsch, Patrick (2015) Retrieval of complex chi((2)) parts for quantitative analysis of sum-frequency generation intensity spectra. JOURNAL OF CHEMICAL PHYSICS, 143 (13): 134112. ISSN 0021-9606, 1089-7690
Full text not available from this repository. (Request a copy)Abstract
Vibrational sum-frequency generation (SFG) spectroscopy has become an established technique for in situ surface analysis. While spectral recording procedures and hardware have been optimized, unique data analysis routines have yet to be established. The SFG intensity is related to probing geometries and properties of the system under investigation such as the absolute square of the second-order susceptibility vertical bar chi((2))vertical bar(2). A conventional SFG intensity measurement does not grant access to the complex parts of chi((2)) unless further assumptions have been made. It is therefore difficult, sometimes impossible, to establish a unique fitting solution for SFG intensity spectra. Recently, interferometric phase-sensitive SFG or heterodyne detection methods have been introduced to measure real and imaginary parts of chi((2)) experimentally. Here, we demonstrate that iterative phase-matching between complex spectra retrieved from maximum entropy method analysis and fitting of intensity SFG spectra (iMEMfit) leads to a unique solution for the complex parts of chi((2)) and enables quantitative analysis of SFG intensity spectra. A comparison between complex parts retrieved by iMEMfit applied to intensity spectra and phase sensitive experimental data shows excellent agreement between the two methods. (C) 2015 AIP Publishing LLC.
| Item Type: | Article |
|---|---|
| Uncontrolled Keywords: | NONLINEAR-OPTICAL SPECTROSCOPY; MAXIMUM-ENTROPY METHOD; VIBRATIONAL SPECTROSCOPY; PHASE MEASUREMENT; SFG-VS; INTERFACES; ORIENTATION; MOLECULES; SURFACES; |
| Subjects: | 500 Science > 540 Chemistry & allied sciences |
| Divisions: | Chemistry and Pharmacy > Institut für Physikalische und Theoretische Chemie |
| Depositing User: | Dr. Gernot Deinzer |
| Date Deposited: | 06 Jun 2019 07:18 |
| Last Modified: | 06 Jun 2019 07:18 |
| URI: | https://pred.uni-regensburg.de/id/eprint/4627 |
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