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Measurement of the nonlinear vibrational spectrum of molecules at a liquid/liquid interface has recently been achieved by the use of total internal reflection sum frequency vibrational spectroscopy (TIR SFVS). This report describes this nonlinear optical technique and gives examples of the type of information which has been obtained about interfacial water and surfactants adsorbed at this interface. The surfactants examined include simple alkyl cationic and anionic surfactants commonly used in cleaning products, and phosphatidylcholines which comprise the major component of cell membranes. Studies of interfacial water involve comparative studies at air/water and oil/water interfaces, and the effect of adsorbed surfactant on the water structure and orientation at these two interfaces.
Work from our laboratory on vibrational sum frequency spectroscopic investigations of molecular ordering at the carbon tetrachloride-water interface is reviewed. Simple charged surfactants adsorbed at the liquid-liquid interface are seen to induce alignment of interfacial water molecules to a degree which is dependent on the induced surface potential. Saturation of water molecule alignment occurs at a surfactant surface concentration corresponding to a calculated surface potential of approximately 160 mV. In complementary studies, the relative degree of hydrocarbon chain ordering within monolayers of symmetric phosphatidylcholines of different chain lengths is inferred by the relative signal contributions of the methyl and methylene symmetric stretch modes. The degree of hydrocarbon chain disorder observed depends strongly on the method of monolayer preparation. By one method, a decrease in hydrocarbon chain order is seen with increasing chain length. Another method of monolayer formation yielded very well ordered hydrocarbon chains for the longest chain phosphatidylcholine studied, and showed much greater disorder in shorter chain species which was comparable to the other preparation method. These studies are a foundation for further work with this technique geared towards understanding molecular-level structural features in membrane-like assemblies and surface biochemical interactions of relevance to biomedical research.
Physical Chemistry of Gas-Liquid Interfaces, the first volume in the Developments in Physical & Theoretical Chemistry series, addresses the physical chemistry of gas transport and reactions across liquid surfaces. Gas–liquid interfaces are all around us, especially within atmospheric systems such as sea spry aerosols, cloud droplets, and the surface of the ocean. Because the reaction environment at liquid surfaces is completely unlike bulk gas or bulk liquid, chemists must readjust their conceptual framework when entering this field. This book provides the necessary background in thermodynamics and computational and experimental techniques for scientists to obtain a thorough understanding of the physical chemistry of liquid surfaces in complex, real-world environments. 2019 PROSE Awards - Winner: Category: Chemistry and Physics: Association of American Publishers Provides an interdisciplinary view of the chemical dynamics of liquid surfaces, making the content of specific use to physical chemists and atmospheric scientists Features 100 figures and illustrations to underscore key concepts and aid in retention for young scientists in industry and graduate students in the classroom Helps scientists who are transitioning to this field by offering the appropriate thermodynamic background and surveying the current state of research
Offers a comprehensive treatment of surface chemistry and its applications to chemical engineering, biology, and medicine. Focuses on the chmical and physical structure of oil-water interfaces and membrane surfaces. Details interfacial potentials, ion solvation, and electrostatic instabilities in double layers.
The advent of laser-based sources of ultrafast infrared pulses has extended the study of very fast molecular dynamics to the observation of processes manifested through their effects on the vibrations of molecules. In addition, non-linear infrared spectroscopic techniques make it possible to examine intra- and intermolecular interactions and how such interactions evolve on very fast time scales, but also in some instances on very slow time scales. Ultrafast Infrared Vibrational Spectroscopy is an advanced overview of the field of ultrafast infrared vibrational spectroscopy based on the scientific research of the leading figures in the field. The book discusses experimental and theoretical topics reflecting the latest accomplishments and understanding of ultrafast infrared vibrational spectroscopy. Each chapter provides background, details of methods, and explication of a topic of current research interest. Experimental and theoretical studies cover topics as diverse as the dynamics of water and the dynamics and structure of biological molecules. Methods covered include vibrational echo chemical exchange spectroscopy, IR-Raman spectroscopy, time resolved sum frequency generation, and 2D IR spectroscopy. Edited by a recognized leader in the field and with contributions from top researchers, including experimentalists and theoreticians, this book presents the latest research methods and results. It will serve as an excellent resource for those new to the field, experts in the field, and individuals who want to gain an understanding of particular methods and research topics.
This coherent collection of theory, algorithms, and illustrative results presents the field of nonequilibrium molecular dynamics in detail.