Consistency in the Sum Frequency Generation Intensity and Phase Vibrational Spectra of the Air/Neat Water Interface

Journal Article · Thu Jun 16 04:00:00 EDT 2011 · Journal of Physical Chemistry A, 115(23):6015-6027

DOI:https://doi.org/10.1021/jp110404h· OSTI ID:1018122

Feng, Ranran; Guo, Yuan; Lu, Rong; Velarde Ruiz Esparza, Luis A; Wang, Hongfei

Tremendous progresses have been made in quantitative understanding and interpretation of the hydrogen bonding and ordering structure at the air/water interface since the first sum-frequency generation vibrational spectroscopy (SFG-VS) measurement on the neat air/water interface by Q. Du et al. in 1993 (PRL, 70, 2312-2316, 1993.). However, there are still disagreements and controversies on the consistency between the different experiment measurements and the theoretical computational results. One critical problem lies in the inconsistency between the SFG-VS intensity measurements and the recently developed SFG-VS phase spectra measurements of the neat air/water interface, which has inspired various theoretical efforts trying to understand them. In this report, the reliability of the SFG-VS intensity spectra of the neat air/water interface is to be quantitatively examined, and the sources of possible inaccuracies in the SFG-VS phase spectral measurement is to be discussed based on the non-resonant SHG phase measurement results. The conclusion is that the SFG-VS intensity spectra data from different laboratories are now quantitatively converging and in agreement with each other, and the possible inaccuracies and inconsistencies in the SFG-VS phase spectra measurements need to be carefully examined against the properly corrected phase standard.

• Research Organization: Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 1018122
• Report Number(s): PNNL-SA-76010; 39892; KP1704020
• Journal Information: Journal of Physical Chemistry A, 115(23):6015-6027, Journal Name: Journal of Physical Chemistry A, 115(23):6015-6027 Journal Issue: 23 Vol. 115
• Country of Publication: United States
• Language: English

Related Subjects

08 HYDROGEN
BONDING
Environmental Molecular Sciences Laboratory
HYDROGEN
RELIABILITY
SFG vibrational spectroscopy
SPECTRA
SPECTROSCOPY
WATER
air/water interface
phase measurement