Biological lipid hydration: distinct mechanisms of interfacial water alignment and charge screening for model lipid membranes.

Studying lipid monolayers as model biological membranes, we demonstrate that water molecules interfacing with different model membranes can display preferential orientation for two distinct reasons: due to charges on the membrane, and due to large dipole fields resulting from zwitterionic headgroups. This preferential water orientation caused by the charge or the dipolar field can be effectively neutralized to net-zero water orientation by introducing monolayer counter-charges ( lipids with oppositely charged headgroups). Following the Gouy-Chapman model, the effect of monolayer surface charge on water orientation is furthermore strongly dependent on the electrolyte concentration and thus on the counterions in solution.

Setup and Analysis of a Mid-Infrared Stand-Off System to Detect Traces of Explosives on Fabrics.

The increasing number of terrorist attacks within the last decade has demonstrated that taking preventive protective measures is highly important. In addition to existing measures, automated detection systems for fast and reliable explosive detection are required. A sensitive spectroscopic system based on mid-infrared spectroscopy has been developed and applied to explosive samples on different types of fabric under various geometric conditions.

Vertically Heterogeneous 2D Semi-Interpenetrating Networks Based on Cellulose Acetate and Cross-Linked Polybutadiene.

This work reports the feasibility of polybutadiene (PB) cross-linking under UV irradiation in the presence of a linear polymer, cellulose acetate (CA), to form semi-interpenetrating polymer networks at the air-water interface. The thermodynamic properties and the morphology of two-dimensional (2D) CA/PB blends are investigated after UV irradiation and for a wide range of CA volume fractions. A contraction of the mixed Langmuir films is observed independent of the composition, in agreement with that recorded for the individual PB monolayer after cross-linking.

Confinement and Cross-Linking of 1,2-Polybutadiene in Two Dimensions at the Air-Water Interface.

Langmuir monolayers of 1,2-polybutadiene (PB) were investigated by means of surface pressure-area isotherms, Brewster angle microscopy (BAM) observations, and sum-frequency generation (SFG) spectroscopy. A homogeneous and stable monolayer is formed 1.5 h after PB spreading provided that both light and oxygen are present.

Unveiling Heterogeneity of Interfacial Water through the Water Bending Mode.

The water bending mode provides a powerful probe of the microscopic structure of bulk aqueous systems because its frequency and spectral line shape are responsive to the intermolecular interactions. Furthermore, interpreting the bending mode response is straightforward, as the intramolecular vibrational coupling is absent. Nevertheless, bending mode has not been used for probing the interfacial water structure, as it has been yet argued that the signal is dominated by bulk effects.

Unraveling the Origin of the Apparent Charge of Zwitterionic Lipid Layers.

The structure of water molecules in contact with zwitterionic lipid molecules is of great biological relevance, because biological membranes are largely composed of such lipids. The interaction of the interfacial water molecules with the amphiphilic lipid molecules drives the formation of membranes and greatly influences various processes at the membrane surface, as the field that arises from the aligned interfacial water molecules masks the charges of the lipid headgroups from the approaching metabolites. To increase our understanding of the influence of water molecules on biological processes we study their structure at the interface using sum-frequency generation spectroscopy and molecular dynamics simulations.

Saturation of charge-induced water alignment at model membrane surfaces.

The electrical charge of biological membranes and thus the resulting alignment of water molecules in response to this charge are important factors affecting membrane rigidity, transport, and reactivity. We tune the surface charge density by varying lipid composition and investigate the charge-induced alignment of water molecules using surface-specific vibrational spectroscopy and molecular dynamics simulations. At low charge densities, the alignment of water increases proportionally to the charge.