相关论文: Intrinsic pH of water/vapor interface revealed by …
Water's ability to autoionize into hydroxide and hydronium ions profoundly influences surface properties, rendering interfaces either basic or acidic. While it is well-established that protons show an affinity to the air-water interface, a…
Molecular-level insight into interfacial water at buried electrode interfaces is essential in elucidating many phenomena of electrochemistry, but spectroscopic probing of the buried interfaces remains challenging. Here, using…
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…
Hydrophobic solid-water interfaces underpin processes in nanofluidics, electrochemistry, and energy technologies. Microscopic insights into these systems are often inferred from our understanding of the air-water interface, which is assumed…
Understanding specific ion adsorption within the inner Helmholtz layer remains central to electrochemistry yet experimentally elusive. Here we directly quantify counterion adsorption and extract the associated thermodynamic parameters…
The magnitude of the pH of the surface of water continues to be a contentious topic in the physical chemistry of aqueous interfaces. Recent theoretical studies have shown little or no preference for the proton to be at the surface compared…
We investigate the properties of water along the liquid/vapor coexistence line in the supercooled regime down to the no-man's land. Extensive molecular dynamics simulations of the TIP4P/2005 liquid/vapor interface in the range 198 -- 348 K…
Understanding the physical and chemical properties of aqueous interfaces is important in diverse fields of science, ranging from biology and chemistry to materials science. In spite of crucial progress in surface sensitive spectroscopic…
The state of protonation/deprotonation of surfaces has far-ranging implications in all areas of chemistry: from acid-base catalysis$^1$ and the electro- and photocatalytic splitting of water$^2$, to the behavior of minerals$^3$ and…
Ion hydration and interfacial water play crucial roles in numerous phenomena ranging from biological to industrial systems. Although biologically relevant (and mostly smaller) ions have been studied extensively in this context, very little…
The preference of water self-ions (hydronium and hydroxide) towards air/oil-water interfaces is one of the hottest topics in water research due to its importance for understanding properties, phenomena, and reactions of interfaces. In this…
Despite widespread interest, a detailed understanding of the dynamics of proton transfer at interfaces is lacking. Here we use ab initio molecular dynamics to unravel the connection between interfacial water structure and proton transfer…
The interactions of a hydrophilic surface with water can significantly influence the characteristics of the liquid water interface. In this manuscript, we explore this influence by studying the molecular structure of liquid water at a…
Anions generally associate more favorably with the air-water interface than cations. In addition to solute size and polarizability, the intrinsic structure of the unperturbed interface has been discussed as an important contributor to this…
The distribution of ions at the air/water interface plays a decisive role in many natural processes. It is generally understood that polarizable ions with low charge density are surface-active, implying they sit on top of the water surface.…
With molecular simulation for water and a tunable hydrophobic substrate, we apply the instantaneous interface construction [A. P. Willard and D. Chandler, J. Phys. Chem. B, 114, 1954 (2010)] to examine the similarity between a water-vapor…
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 compute ionic free energy adsorption profiles at aqueous graphene interface by developing a self-consistent approach. To do so, we design a microscopic model for water and put the liquid on an equal footing with the graphene described by…
Sum frequency generation vibrational spectra of the water molecules at the NaF and KF aqueous solution surfaces showed significantly different spectral features and different concentration dependence. This result is the first direct…
The adsorption behavior of ions at liquid-vapor interfaces exhibits several unexpected yet generic features. In particular, energy and entropy are both minimum when the solute resides near the surface, for a variety of ions in a range of…