Sum-Frequency Generation at Second Order in Isotropic Chiral Systems: The Microscopic View and the Surprising Fragility of the Signal

2002 ◽  
pp. 130-144 ◽  
Author(s):  
Jason Kirkwood ◽  
A. C. Albrecht ◽  
Peer Fischer ◽  
A. D. Buckingham
Keyword(s):  
Sum Frequency Generation ◽  
Second Order ◽  
Sum Frequency ◽  
Frequency Generation ◽  
Chiral Systems

Bulk Contributions Modulate the Sum-Frequency Generation Spectra of Interfacial Water on Model Sea-Spray Aerosols

2018 ◽  
Author(s):  
Sandeep K. Reddy ◽  
Raphael Thiraux ◽  
Bethany A. Wellen Rudd ◽  
Lu Lin ◽  
Tehseen Adel ◽  
...  
Keyword(s):  
Single Layer ◽  
Sum Frequency Generation ◽  
Second Order ◽  
Interfacial Structure ◽  
Sea Spray ◽  
Third Order ◽  
Systematic Analysis ◽  
Sum Frequency ◽  
Structure Of Water ◽  
Frequency Generation

Vibrational sum-frequency generation (vSFG) spectroscopy is used to determine the molecular structure of water at the interface of palmitic acid monolayers. Both measured and calculated spectra display speci c features due to third-order contributions to the vSFG response which are associated with nite interfacial electric potentials. We demonstrate that theoretical modeling enables to separate the third-order contributions, thus allowing for a systematic analysis of the strictly surface-sensitive, second-order component of the vSFG response. This study provides fundamental, molecular-level insights into the interfacial structure of water in a neutral surfactant system with relevance to single layer bio-membranes and environmentally relevant sea-spray aerosols. These results emphasize the key role that computer simulations can play in interpreting vSFG spectra and revealing microscopic details of water at complex interfaces, which can be difficult to extract from experiments due to the mixing of second-order, surface-sensitive and third-order, bulk-dependent contributions to the vSFG response.

Second-order sum-frequency generation in sodium vapor

1976 ◽  
Vol 18 (2) ◽  
pp. 223 ◽  
Author(s):  
D.S. Bethune ◽  
R.W. Smith ◽  
Y.R. Shen
Keyword(s):  
Sum Frequency Generation ◽  
Second Order ◽  
Sodium Vapor ◽  
Sum Frequency ◽  
Frequency Generation

Molecular interactions of organic molecules at the air/water interface investigated by sum frequency generation vibrational spectroscopy

2017 ◽  
Vol 19 (6) ◽  
pp. 4488-4493 ◽  
Author(s):  
Wenting Wang ◽  
Shuji Ye
Keyword(s):  
Vibrational Spectroscopy ◽  
Molecular Interactions ◽  
Organic Molecules ◽  
Sum Frequency Generation ◽  
Second Order ◽  
Water Interface ◽  
Sum Frequency ◽  
Air Water Interface ◽  
Frequency Generation

Second-order Fermi resonanance interaction provides an effective vibrational optical ruler for characterizing the molecular interactions at interfaces.

Bulk Contributions Modulate the Sum-Frequency Generation Spectra of Interfacial Water on Model Sea-Spray Aerosols

2018 ◽  
Author(s):  
Sandeep K. Reddy ◽  
Raphael Thiraux ◽  
Bethany A. Wellen Rudd ◽  
Lu Lin ◽  
Tehseen Adel ◽  
...  
Keyword(s):  
Single Layer ◽  
Sum Frequency Generation ◽  
Second Order ◽  
Interfacial Structure ◽  
Sea Spray ◽  
Third Order ◽  
Systematic Analysis ◽  
Sum Frequency ◽  
Structure Of Water ◽  
Frequency Generation

Vibrational sum-frequency generation (vSFG) spectroscopy is used to determine the molecular structure of water at the interface of palmitic acid monolayers. Both measured and calculated spectra display speci c features due to third-order contributions to the vSFG response which are associated with nite interfacial electric potentials. We demonstrate that theoretical modeling enables to separate the third-order contributions, thus allowing for a systematic analysis of the strictly surface-sensitive, second-order component of the vSFG response. This study provides fundamental, molecular-level insights into the interfacial structure of water in a neutral surfactant system with relevance to single layer bio-membranes and environmentally relevant sea-spray aerosols. These results emphasize the key role that computer simulations can play in interpreting vSFG spectra and revealing microscopic details of water at complex interfaces, which can be difficult to extract from experiments due to the mixing of second-order, surface-sensitive and third-order, bulk-dependent contributions to the vSFG response.

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