相关论文: Both Inter- and Intramolecular Coupling of O-H Gro…
The unique structural properties of interfacial water are at the heart of a vast range of important processes in electrochemistry, climate science, and biophysics. At interfaces, water molecules exhibit preferential orientations and an…
Fluids under extreme confinement exhibit unique structures and intermolecular bonding, distinct from their bulk analogs, driving innovative applications at the water-energy nexus. Probing confined water experimentally at the length scale of…
We simulate vibrational strong (VSC) and ultrastrong coupling (V-USC) for liquid water with classical molecular dynamics simulations. When the cavity modes are resonantly coupled to the O-H stretch mode of liquid water, the infrared…
One of the most popular subjects now being researched in molecular science is strong light-matter coupling. The introduction of vibrational strong coupling and the formation vibro-polaritonic states tend to modify chemical reactivity,…
Water is an ubiquitous liquid that has several exotic and anomalous properties. Despite its apparent simple chemical formula, its capability of forming a dynamic network of hydrogen bonds leads to a rich variety of physics. Here we study…
We have applied path integral molecular dynamics simulations to investigate nuclear quantum effects on the vibrational dynamics of water molecules at the water-air interface. The instantaneous fluctuations in the frequencies of the O-H…
We model, simulate, and analyze the intramolecular modes of liquid H2O and D2O to elucidate how energy excitation, relaxation, and vibrational dephasing interplay through anharmonic mode-mode coupling. Our analysis employs two-dimensional…
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…
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…
Water is an important molecule in interstellar and circumstellar environments. Previous observations of mid-infrared rotational lines of OH suggest that these lines may be used to probe the photodissociation of water. In this work, cross…
Recent experiments have demonstrated that vibrational strong coupling (VSC) between molecular vibrations and the optical cavity field can modify vibrational energy transfer (VET) processes in molecular systems. However, the underlying…
The interplay between intra-molecular H-O covalent bond contraction, due to molecular under-coordination, and inter-molecular O:H expansion, due to inter-electron pair Coulomb repulsion, has been shown to be the source of the anomalous…
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…
Based on quantum-mechanical path-integral molecular dynamics simulations the impact of nuclear quantum effects on the vibrational and hydrogen bond dynamics in liquid water is investigated. The instantaneous fluctuations in the frequencies…
Electron coupling to intra- and inter-molecular vibrational modes is investigated in models appropriate to single crystal organic semiconductors, such as oligoacenes. Focus is on spectral and transport properties of these systems beyond…
To investigate the possibility of measuring the intermolecular and intramolecular anharmonic coupling of balk water, we calculate third-order two-dimensional (2D) infrared (IR) spectra and fifth-order 2D IR-IR-Raman-Raman spectra expressed…
Vibrational spectroscopy is key for probing the interplay between the structure and dynamics of aqueous systems. In order to map different regions of experimental spectra to the microscopic structure of a system, it is important to combine…
We report vibrational sum frequency generation spectra from supported lipid bilayers in which the OH and the CH stretching signals are probed at different salt concentrations. Atomistic simulations show a negligible impact of salt on the OH…
We explore by means of modeling how absorptive-dispersive mixing between the second- and third-order terms modify the imaginary chi(2)total responses from air/water interfaces under conditions of varying charge densities and ionic strength.…
Molecular dynamics simulations of supercritical water reveal distinctly different distance-dependent modulations of dipolar response and correlations in particle motion compared to ambient conditions. The strongly perturbed H-bond network…