scholarly journals “On-The-Fly” Calculation of the Vibrational Sum-Frequency Generation Spectrum at the Air-Water Interface

Molecules ◽  
2020 ◽  
Vol 25 (17) ◽  
pp. 3939 ◽  
Author(s):  
Deepak Ojha ◽  
Thomas D. Kühne
Keyword(s):  
Low Frequency ◽  
Sum Frequency Generation ◽  
Water Interface ◽  
Wannier Functions ◽  
Sum Frequency ◽  
Generation Spectrum ◽  
Air Water Interface ◽  
Bond Stretching ◽  
Frequency Generation

In the present work, we provide an electronic structure based method for the “on-the-fly” determination of vibrational sum frequency generation (v-SFG) spectra. The predictive power of this scheme is demonstrated at the air-water interface. While the instantaneous fluctuations in dipole moment are obtained using the maximally localized Wannier functions, the fluctuations in polarizability are approximated to be proportional to the second moment of Wannier functions. The spectrum henceforth obtained captures the signatures of hydrogen bond stretching, bending, as well as low-frequency librational modes.

scholarly journals “On-the-fly” calculation of the Vibrational Sum-frequency Generation Spectrum at the Air-water Interface

2020 ◽  
Author(s):  
Deepak Ojha ◽  
Thomas Kühne
Keyword(s):  
Predictive Power ◽  
Low Frequency ◽  
Sum Frequency Generation ◽  
Water Interface ◽  
Wannier Functions ◽  
Sum Frequency ◽  
Generation Spectrum ◽  
Air Water Interface ◽  
Bond Stretching ◽  
Frequency Generation

In the present work, we provide an electronic structure based method for the “on-the-fly” deter- mination of vibrational sum frequency generation (v-SFG) spectra. The predictive power of this scheme is demonstrated at the air-water interface. While the instantaneous fluctuations in dipole moment are obtained using the maximally localized Wannier functions, the fluctuations in polar- izability are approximated to be proportional to the second moment of Wannier functions. The spectrum henceforth obtained captures the signatures of hydrogen bond stretching, bending, as well as low-frequency librational modes.

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>

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>

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.

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>

scholarly journals Molecular rotation in 3 dimensions at an air/water interface using femtosecond time resolved sum frequency generation

2019 ◽  
Vol 150 (9) ◽  
pp. 094709 ◽  
Author(s):  
Yi Rao ◽  
Yuqin Qian ◽  
Gang-Hua Deng ◽  
Ashlie Kinross ◽  
Nicholas J. Turro ◽  
...  
Keyword(s):  
Sum Frequency Generation ◽  
Molecular Rotation ◽  
Water Interface ◽  
Time Resolved ◽  
Sum Frequency ◽  
Air Water Interface ◽  
Frequency Generation

Duramycin-Induced Destabilization of a Phosphatidylethanolamine Monolayer at the Air−Water Interface Observed by Vibrational Sum-Frequency Generation Spectroscopy

Langmuir ◽  
2010 ◽  
Vol 26 (20) ◽  
pp. 16055-16062 ◽  
Author(s):  
Izabela I. Rzeźnicka ◽  
Maria Sovago ◽  
Ellen H. G. Backus ◽  
Mischa Bonn ◽  
Taro Yamada ◽  
...  
Keyword(s):  
Sum Frequency Generation ◽  
Water Interface ◽  
Sum Frequency ◽  
Sum Frequency Generation Spectroscopy ◽  
Air Water Interface ◽  
Frequency Generation
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