Analysis of surface second-harmonic generation by orientational distribution function in a chiral polymer film

Abstract

By adopting classical models of molecular chirality, contributions of the coupled-oscillator and helix natures to the chiral surface second-order susceptibilities are identified through introduction of a molecular orientational distribution. Experimentally, surface orientational distribution functions at interfaces of an isotropic chiral chitosan polymer film are determined from second harmonic generation measurement. The largest chiral component of surface nonlinear optical susceptibility is from the electric-magnetic coupling with dominant contribution from the helix nature of chitosan. © 2005 The American Physical Society.