Abstract

ABSTRACTPolymeric films fabricated from ionically self-assembled monolayers (ISAMs) spontaneously form in a noncentrosymmetric structure requisite for a nonzero second order nonlinear optical (NLO) susceptibility, without the need for electric field poling. ISAM NLO films exhibit excellentlong-term temporal stability of having shown no decay over a period of nearly three years. Theyare also remarkably stable at elevated temperatures. While decreases by 20% as the temperatureis raised to 150° C, total recovery of the susceptibility is observed upon cooling, demonstrating thatthe decrease is not due to an irreversible randomization of the chromophore alignment. The thickness,onentational order, and NLO response are found to be strongly dependent on the pH and ionic strength of the solutions from which the films are deposited. The largest values are observed infilms with the smallest bilayer thickness. This suggests that polar orientation is obtained primarily atthe interfaces between adjacent layers rather than throughout a full monolayer.Keywords: second order nonlinear optical susceptibility, ionically self-assembled monolayers,thermal stability, pH, ionic strength1. INTRODUCTION

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