Orientations of nonlocal vibrational modes from combined experimental and theoretical sum frequency spectroscopy

Journal Article · Fri Sep 01 04:00:00 EDT 2017 · Chemical Physics Letters

DOI:https://doi.org/10.1016/j.cplett.2017.01.015· OSTI ID:1378004

Chase, Hilary M.; Chen, Shunli; Fu, Li; Upshur, Mary Alice; Rudshteyn, Benjamin; Thomson, Regan J.; Wang, Hong-Fei; Batista, Victor S.; Geiger, Franz M.

Inferring molecular orientations from vibrational sum frequency generation (SFG) spectra is challenging in polarization combinations that result in low signal intensities, or when the local point group symmetry approximation fails. While combining experiments with density functional theory (DFT) could overcome this problem, the scope of the combined method has yet to be established. Here, we assess its feasibility of determining the distributions of molecular orientations for one monobasic ester, two epoxides and three alcohols at the vapor/fused silica interface. We find that molecular orientations of nonlocal vibrational modes cannot be determined using polarization-resolved SFG measurements alone.

• Research Organization: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 1378004
• Report Number(s): PNNL-SA--122921; 49672; 49291; KP1704020
• Journal Information: Chemical Physics Letters, Journal Name: Chemical Physics Letters Journal Issue: C Vol. 683; ISSN 0009-2614
• Publisher: Elsevier
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Environmental Molecular Sciences Laboratory