Bend Vibration of Surface Water Investigated by Heterodyne-Detected Sum Frequency Generation and Theoretical Study: Dominant Role of Quadrupole

Kundu, Achintya; Tanaka, Shogo; Ishiyama, Tatsuya; Ahmed, Mohammed; Inoue, Ken; Nihonyanagi, Satoshi; Sawai, Hiromi; Yamaguchi, S.; Morita, Akihiro; Tahara, Tahei

doi:10.1021/acs.jpclett.6b00657

Cited by 56 publications

(92 citation statements)

References 48 publications

(113 reference statements)

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“…The experiments are typically performed by adding small amounts of µM lipid solutions to ultrapure water contained in a Langmuir trough. In heterodyned, or phase-sensitive, SFG spectra, the sign of the Im(χ (2) ) is commonly taken to indicate an "up" or "down" orientation of the OH oscillators that are probed [28][29][30] . Indeed, Figs.…”

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confidence: 99%

Second-order spectral lineshapes from charged interfaces

2017

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Second-order nonlinear spectroscopy has proven to be a powerful tool in elucidating key chemical and structural characteristics at a variety of interfaces. However, the presence of interfacial potentials may lead to complications regarding the interpretation of second harmonic and vibrational sum frequency generation responses from charged interfaces due to mixing of absorptive and dispersive contributions. Here, we examine by means of mathematical modeling how this interaction influences second-order spectral lineshapes. We discuss our findings in the context of reported nonlinear optical spectra obtained from charged water/air and solid/liquid interfaces and demonstrate the importance of accounting for the interfacial potential-dependent χ (3) term in interpreting lineshapes when seeking molecular information from charged interfaces using second-order spectroscopy.

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confidence: 99%

Second-order spectral lineshapes from charged interfaces

2017

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“…In principle, when the input IR beam is p-polarized, the sign of the frequency-dependent amplitude of Im(χ (2) ) spectra informs on whether the z-component of the transition dipole moment in a given oscillator Ohno et al 3 contributing to the SFG spectrum is directed net "up" or net "down". 27 Yet, as we will show, in the presence of interfacial charge, crossovers between positive and negative regions can occur, not caused by changes in orientation of interfacial molecules, but rather produced by χ (2) /χ (3) mixing.…”

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confidence: 61%

Second-Order Vibrational Lineshapes from the Air/Water Interface

et al. 2018

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We explore by means of modeling how absorptive-dispersive mixing between the second- and third-order terms modifies the imaginary χ responses from air/water interfaces under conditions of varying charge densities and ionic strength. To do so, we use published Im(χ) and χ spectra of the neat air/water interface that were obtained either from computations or experiments. We find that the χ spectral lineshapes corresponding to experimentally measured spectra contain significant contributions from both interfacial χ and bulk χ terms at interfacial charge densities equivalent to less than 0.005% of a monolayer of water molecules, especially in the 3100 to 3300 cm frequency region. Additionally, the role of short-range static dipole potentials is examined under conditions mimicking brine. Our results indicate that surface potentials, if indeed present at the air/water interface, manifest themselves spectroscopically in the tightly bonded H-bond network observable in the 3200 cm frequency range.

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“…There have been theoretical calculations predicting significant quadrupole contributions to surface susceptibilities for liquid benzene and water surfaces [162,163]. For the water bending mode at the air/water interface, calculation indicates that the bulk quadrupole contributions are 8.7 times of that for the surface dipole contribution [163].…”

Section: Surface and Bulk Contributions In Sfg-vsmentioning

confidence: 99%

Sum frequency generation vibrational spectroscopy (SFG-VS) for complex molecular surfaces and interfaces: Spectral lineshape measurement and analysis plus some controversial issues

Wang

2016

Progress in Surface Science

105

127

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Sum-frequency generation vibrational spectroscopy (SFG-VS) was first developed in the 1980s and it has been proven a uniquely sensitive and surface/interface selective spectroscopic probe for characterization of the structure, conformation and dynamics of molecular surfaces and interfaces. In recent years, there have been many progresses in the development of methodology and instrumentation in the SFG-VS toolbox that has significantly broadened the application to complex molecular surfaces and interfaces. In this review, after presenting a unified view on the theory and methodology focusing on the SFG-VS spectral lineshape, as well as the new opportunities in SFG-VS applications with such developments, some of the controversial issues that have been puzzling the community are discussed. The aim of this review is to present to the researchers and students interested in molecular surfaces and interfacial sciences up-to-date perspectives complementary to the existing textbooks and reviews on SFG-VS.

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Bend Vibration of Surface Water Investigated by Heterodyne-Detected Sum Frequency Generation and Theoretical Study: Dominant Role of Quadrupole

Cited by 56 publications

References 48 publications

Second-order spectral lineshapes from charged interfaces

Second-order spectral lineshapes from charged interfaces

Second-Order Vibrational Lineshapes from the Air/Water Interface

Sum frequency generation vibrational spectroscopy (SFG-VS) for complex molecular surfaces and interfaces: Spectral lineshape measurement and analysis plus some controversial issues

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