Related papers: Polarization and Experimental Configuration Analys…
Analysis of SFG vibrational spectra of OH stretching bands in four experimental configurations shows that orientational motion of water molecule at air/water interface is libratory within a limited angular range. This picture is…
The air-water and graphene-water interfaces represent quintessential examples of the liquid-gas and liquid-solid boundaries, respectively. While the sum-frequency generation (SFG) spectra of these interfaces exhibit certain similarities, a…
Interface-specific hydrogen- (H-)bonding network of water next to a substrate (including air) directly controls the energy transfer and chemical reaction pathway at many charged aqueous interfaces. Yet, experimental characterization of such…
In order to understand the nature and dynamics of interfacial water molecules on the surface of complex systems, large scale molecular dynamics simulations of an aqueous micelle of cesium perfluorooctanoate surfactant molecules have been…
The interpretation of sum-frequency-generation (SFG) spectra has been severely limited by the absence of quantitative theoretical predictions of higher-order multipole contributions. Magnetic dipole and electric quadrupole contributions are…
The air-water interface is a highly prevalent phase boundary with a far-reaching impact on natural and industrial processes. Water molecules behave differently at the interface compared to the bulk, exhibiting anisotropic orientational…
Most properties of liquid water are determined by its hydrogen-bond network. Because forming an aqueous interface requires termination of this network, one might expect the molecular level properties of interfacial water to markedly differ…
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.…
It has been generally accepted that there are significant quadrupolar and bulk contributions to the second harmonic generation (SHG) reflected from the neat air/water interface, as well as common liquid interfaces. Because there has been no…
Understanding the molecular-level structure and dynamics of ice surfaces is crucial for deciphering several chemical, physical, and atmospheric processes. Vibrational sum-frequency generation (SFG) spectroscopy is the most prominent tool…
The molecular water structure at charged aqueous interfaces is shaped by interfacial electric fields, which can induce significant anisotropy in the molecular orientations extending over nanometer-scale distances. Despite great relevance,…
Much work over the last 25 years has demonstrated that the interface-specific, alloptical technique, vibrational sum frequency generation (v-SFG) spectroscopy, is often uniquely capable of characterizing the structure and dynamics of…
Magnetite, a naturally abundant mineral, frequently interacts with water in both natural settings and various technical applications, making the study of its surface chemistry highly relevant. In this work, we investigate the hydrogen…
In a recent letter (PRL,121,246101,2018), Sun et al. reported that combined MD simulation and sum frequency generation vibrational spectroscopy (SFG-VS) measurements led to conclusions of a broad and exponentially decaying orientational…
Water plays a crucial role in geological, biological, and technological processes. Nanoscale water confinement occurs in many of these settings, including sedimentary rocks, water channel proteins, and applications like desalination and…
Protons at the water/vapor interface are relevant for atmospheric and environmental processes, yet to characterize their surface affinity on the quantitative level is still challenging. Here we utilize phase-sensitive sum-frequency…
Path-integral molecular dynamics simulations and electronic structure-based energy decomposition analysis (EDA) are employed to connect hydrogen bond (H-bond) strength, its asymmetry, and the total delocalization energy at the water/air…
We have developed x-ray diffraction measurements with high energy-resolution and accuracy to study water structure at three different temperatures (7, 25 and 66 C) under normal pressure. Using a spherically curved Ge crystal an energy…
The Surface Green Function Matching analysis (SGFM) is used to study the normal modes of the interface oscillations between two non-mixed fluids by considering the difference in their densities and viscosities. The limiting case of…
The local structure of liquid water as a function of temperature is a source of intense research. This structure is intimately linked to the dynamics of water molecules, which can be measured using Raman and infrared spectroscopies. The…