Sum-frequency generation first hyperpolarizability from time-dependent Hartree-Fock method

2001 ◽  
Vol 85 (4-5) ◽  
pp. 463-468 ◽  
Author(s):  
Olivier Quinet ◽  
Beno�t Champagne
Keyword(s):  
Sum Frequency Generation ◽  
Time Dependent ◽  
First Hyperpolarizability ◽  
Sum Frequency ◽  
Hartree Fock ◽  
Frequency Generation

scholarly journals Time-dependent vibrational sum-frequency generation spectroscopy of the air-water interface

2019 ◽  
Vol 2 (1) ◽  
Author(s):  
Deepak Ojha ◽  
Naveen Kumar Kaliannan ◽  
Thomas D. Kühne
Keyword(s):  
Sum Frequency Generation ◽  
Time Dependent ◽  
Water Molecules ◽  
Water Interface ◽  
Sum Frequency ◽  
Generation Spectrum ◽  
Structure And Dynamics ◽  
Sum Frequency Generation Spectroscopy ◽  
Air Water Interface ◽  
Frequency Generation

Abstract Vibrational sum-frequency generation spectroscopy is a powerful method to study the microscopic structure and dynamics of interfacial systems. Here we demonstrate a simple computational approach to calculate the time-dependent, frequency-resolved vibrational sum-frequency generation spectrum (TD-vSFG) of the air-water interface. Using this approach, we show that at the air-water interface, the transition of water molecules with bonded OH modes to free OH modes occurs at a time scale of $$\sim$$ ~ 3 ps, whereas water molecules with free OH modes rapidly make a transition to a hydrogen-bonded state within $$\sim$$ ~ 2 ps. Furthermore, we also elucidate the origin of the observed differential dynamics based on the time-dependent evolution of water molecules in the different local solvent environments.

An in Situ Time-Dependent Study of CO Oxidation on Pt(111) in Aqueous Solution by Voltammetry and Sum Frequency Generation

2003 ◽  
Vol 107 (8) ◽  
pp. 1840-1844 ◽  
Author(s):  
Keng C. Chou ◽  
Nenad M. Markovic ◽  
Joonyeong Kim ◽  
Philip N. Ross ◽  
Gabor A. Somorjai
Keyword(s):  
Aqueous Solution ◽  
Co Oxidation ◽  
Sum Frequency Generation ◽  
Time Dependent ◽  
Sum Frequency ◽  
Frequency Generation

Temperature Dependence of the Air/Water Interface Revealed by Polarization Sensitive Sum-Frequency Generation Spectroscopy

2018 ◽  
Author(s):  
Daniel R. Moberg ◽  
Shelby C. Straight ◽  
Francesco Paesani
Keyword(s):  
Temperature Dependence ◽  
Low Frequency ◽  
Potential Energy Function ◽  
Md Simulations ◽  
Sum Frequency Generation ◽  
Water Molecules ◽  
Water Interface ◽  
Sum Frequency ◽  
Air Water Interface ◽  
Frequency Generation

<div> <div> <div> <p>The temperature dependence of the vibrational sum-frequency generation (vSFG) spectra of the the air/water interface is investigated using many-body molecular dynamics (MB-MD) simulations performed with the MB-pol potential energy function. The total vSFG spectra calculated for different polarization combinations are then analyzed in terms of molecular auto-correlation and cross-correlation contributions. To provide molecular-level insights into interfacial hydrogen-bonding topologies, which give rise to specific spectroscopic features, the vSFG spectra are further investigated by separating contributions associated with water molecules donating 0, 1, or 2 hydrogen bonds to neighboring water molecules. This analysis suggests that the low frequency shoulder of the free OH peak which appears at ∼3600 cm−1 is primarily due to intermolecular couplings between both singly and doubly hydrogen-bonded molecules. </p> </div> </div> </div>

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.

Sum Frequency Generation Vibrational Spectroscopy of 1,3-Butadiene Hydrogenation on 4 nm Pt@SiO2, Pd@SiO2, and Rh@SiO2 Core–Shell Catalysts

Nano Letters ◽  
2014 ◽  
Vol 15 (1) ◽  
pp. 39-44 ◽  
Author(s):  
James M. Krier ◽  
William D. Michalak ◽  
Xiaojun Cai ◽  
Lindsay Carl ◽  
Kyriakos Komvopoulos ◽  
...  
Keyword(s):  
Vibrational Spectroscopy ◽  
Sum Frequency Generation ◽  
Core Shell ◽  
Sum Frequency ◽  
Frequency Generation ◽  
Butadiene Hydrogenation
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