Optical manipulation of third-harmonic generation via either one- or two-photon excitation in diarylethene-polymethylmethacrylate polymer thin films

Abstract

Optical manipulation of third harmonic (TH) generation in diarylethene-polymethylmethacrylate (DE-PMMA) polymer thin films is obtained by either one- or two-photon excitation. TH intensity generated from a DE-PMMA polymer thin film decreases, when it is pumped by either 325 nm or 442 nm laser irradiation, which changes the molecular structure of DE molecules from an open-form (A form) to a closed-form (B form). TH intensity recovers to its original intensity level when all B form DE molecules return to an A form after being induced by either 532 nm or 1064 nm laser irradiation. The experimental results reveal that the second-order hyperpolarizability (γ) of the A form molecules may be larger than that of the B form molecules. Moreover, TH output efficiency is independent of the angle between the pump and probe polarization directions. This result is attributed to the two-dimensional structure of DE molecules.