Charge generation and separation at liquid interfaces. Technical progress report

摘要

The research is divided into 3 parts: (1)Sum Frequency Generation (SFG) and Monolayer Structure. Picosecond lasers are combined by difference frequency mixing in a nonlinear crystal to generate picosecond, tunable IR pulses, which are used to study orientation of C(double bond)N and CD(sub 3) chromosphores (head group and tail) on lipid monolayers CD(sub 3)(CH(sub 2))(sub 21)CN at air /water interface. (2)Femtosecond Dynamics. The femtosecond colliding pulse mode locked laser is being modified to carry out pump-second harmonic (SH) probe studies at liquid interfaces. Picosecond SH knowhow of intermolecular energy transfer, excited state isomerization, and rotational motions at interfaces is now being applied to femtosecond scale. Aromatics adsorbed at air /water interface, generated changes in SH probe signal and their decay back to original value. If the laser is tightly focussed at interface, multiphoton absorption processes occur which destroy the sample; this effect will be exploited. (3)Interface Potential and Acid-Base Equilibria. The interface potential is a key to charge transport; using SHG, we plan to measure the pKa of organic acids at interfaces. In these studies at silica/aqueous interface, the water molecules extending from the interface into the bulk (about 50(Angstrom)) were strongly polarized by SiO(sup (minus)) charges at the interface. In summary, a new spectroscopic technique is being applied to study of neutral and charged lipid monolayers, interface pKa values, interface potential and orientational structure and vibrational spectroscopy of lipids.