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  4. Second Harmonic and Sum-Frequency Generation from Aqueous Interfaces Is Modulated by Interference
 
research article

Second Harmonic and Sum-Frequency Generation from Aqueous Interfaces Is Modulated by Interference

Gonella, Grazia
•
Luetgebaucks, Cornelis  
•
De Beer, Alex G. F.
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2016
Journal Of Physical Chemistry C

The interfacial region of aqueous systems also known as the electrical double layer can be characterized on the molecular level with second harmonic and sum-frequency generation (SHG/SFG). SHG and SFG are surface specific methods for isotropic liquids. Here, we model the SHG/SFG intensity in reflection, transmission, and scattering geometry taking into account the spatial variation of all fields. We show that, in the presence of a surface electrostatic field, interference effects, which originate from oriented water molecules on a length scale over which the potential decays, can strongly modify the probing depth as well as the expected intensity at ionic strengths <10(-3) M. For reflection experiments this interference phenomenon leads to a significant reduction of the SHG/SFG intensity. Transmission mode experiments from aqueous interfaces are hardly influenced. For SHG/SFG scattering experiments the same interference leads to an increase in intensity and to modified scattering patterns. The predicted scattering patterns are verified experimentally.

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Type
research article
DOI
10.1021/acs.jpcc.5b12453
Web of Science ID

WOS:000375631100018

Author(s)
Gonella, Grazia
Luetgebaucks, Cornelis  
De Beer, Alex G. F.
Roke, Sylvie  
Date Issued

2016

Publisher

American Chemical Society

Published in
Journal Of Physical Chemistry C
Volume

120

Issue

17

Start page

9165

End page

9173

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LBP  
Available on Infoscience
July 19, 2016
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/127730
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