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Title: Potential modulation of equilibrium and excitation phenomena at the electrolyte-solid interface

This progress report covers the work accomplished from the beginning of Sept. 1990, through Sept. 1991. This includes the final portion of the last funding period as well as the first 7 months of the new period. During this time we have pursued our goal of studying the role of the interfacial potential difference in determining the ground and excited electronic sates of the electrolyte-solid system. Ours is program designed to provide fundamental information about this complicated environment. We seek to improve the techniques with which electrochemical interfaces can be studied and thereby observe details which have never before been measured. We are primarily concerned with optical techniques, but have also integrated conventional and non-conventional supplementary methods. We have developed the technique of optical second harmonic generation into a spectroscopy by performing the experiment with a wide range of nearly continuous incident photon energies. Through this advantage we have performed detailed tests of the interfacial potential as derived through local density functional methods in the jellium limit. Our data show that the theory is reasonably satisfactory when the surface is electron deficient. However, when the surface is negatively charged (electron excess) significant discrepancies are evident. At least part of thismore » deviation has been explained by transitions involving potential modulated surface states. This project has helped clarify some important questions concerning the nonlinear optical properties of metals, as well as lay he ground work for future applications aimed at monitoring adsorption phenomena with optical second harmonic reflectance spectroscopy.« less
Authors:
Publication Date:
OSTI Identifier:
6250728
Report Number(s):
DOE/ER/45253-6
ON: DE92003453
DOE Contract Number:
FG02-86ER45253
Resource Type:
Technical Report
Research Org:
Colorado School of Mines, Golden, CO (United States). Dept. of Physics
Sponsoring Org:
DOE; USDOE, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ELECTRODES; INTERFACES; ELECTROLYTES; EXCITED STATES; GROUND STATES; MICROBALANCES; PROGRESS REPORT; SAMPLE PREPARATION; SILVER; SPECTROSCOPY; BALANCES; DOCUMENT TYPES; ELEMENTS; ENERGY LEVELS; MEASURING INSTRUMENTS; METALS; TRANSITION ELEMENTS; WEIGHT INDICATORS 400400* -- Electrochemistry