Ordering of Interfacial Water Molecules at the Charged Air/Water Interface Observed by Vibrational Sum 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>

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

10.26434/chemrxiv.5938177 ◽

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>

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

Communications Chemistry ◽

10.1038/s42004-019-0220-6 ◽

2019 ◽

Vol 2 (1) ◽

Cited By ~ 6

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.

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

10.26434/chemrxiv.5938177.v1 ◽

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>

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Investigation of the interfacial water structure on poly[2-(dimethylamino)ethyl methacrylate] at the air/water interface by sum frequency generation vibrational spectroscopy

Chinese Science Bulletin ◽

10.1007/s11434-011-4963-4 ◽

2012 ◽

Vol 57 (9) ◽

pp. 984-991 ◽

Cited By ~ 1

Author(s):

Dan Wu ◽

Yuan Guo ◽

GuangMing Liu ◽

GuangZhao Zhang

Keyword(s):

Vibrational Spectroscopy ◽

Water Structure ◽

Sum Frequency Generation ◽

Interfacial Water ◽

Water Interface ◽

Sum Frequency ◽

Ethyl Methacrylate ◽

Air Water Interface ◽

Frequency Generation ◽

Interfacial Water Structure

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The structure of a lanthanide complex at an extractant/water interface studied using heterodyne-detected vibrational sum frequency generation

Physical Chemistry Chemical Physics ◽

10.1039/c7cp06758e ◽

2018 ◽

Vol 20 (4) ◽

pp. 2809-2813 ◽

Cited By ~ 5

Author(s):

Ryoji Kusaka ◽

Masayuki Watanabe

Keyword(s):

Lanthanide Complex ◽

Sum Frequency Generation ◽

Water Molecules ◽

Water Interface ◽

Lower Side ◽

Sum Frequency ◽

Frequency Generation

Eu3+ at an extractant/water interface is bound to extractants from the upper side and to water molecules from the lower side, and forms a unique interfacial complex.

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