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

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.

[1]  Satoshi Kawata,et al.  The Photoorientation Movement of a Diarylethene-Type Chromophore , 2000 .

[2]  Fumihiro Ebisawa,et al.  Refractive index change in photochromic diarylethene derivatives and its application to optical switching devices , 1997 .

[3]  Satoshi Kawata,et al.  Two-photon isomerization and orientation of photoisomers in thin films of polymer , 2003 .

[4]  Zouheir Sekkat,et al.  Photoreactive organic thin films , 2002 .

[5]  Michel Dumont,et al.  Photoinduced orientation of azo dyes in polymeric films. Characterization of molecular angular mobility , 1993 .

[6]  Masahiro Irie,et al.  Diarylethenes for Memories and Switches. , 2000, Chemical reviews.

[7]  Chia Chen Hsu,et al.  Optical control of third-harmonic generation in azo-doped polymethylmethacrylate thin films , 2000 .

[8]  Hidemitsu Furukawa,et al.  Photochemically Induced Fluorescence Control with Intermolecular Energy Transfer from a Fluorescent Dye to a Photochromic Diarylethene in a Polymer Film , 2003 .

[9]  Jacques A. Delaire,et al.  Nonlinear Optical Properties of Diarylethenes , 2000 .

[10]  Masahiro Irie,et al.  Thermally irreversible photochromic systems. Reversible photocyclization of diarylethene derivatives , 1988 .

[11]  S. Kobatake,et al.  Reversible surface morphology changes of a photochromic diarylethene single crystal by photoirradiation. , 2001, Science.

[12]  Z. Sekkat.  Isomeric orientation by two-photon excitation: a theoretical study , 2004 .

[13]  He Tian,et al.  Recent progresses on diarylethene based photochromic switches. , 2004, Chemical Society reviews.

[14]  Zouheir Sekkat,et al.  Observation of Reversible Photochemical “Blow Out” of the Third-Order Molecular Hyperpolarizability of Push−Pull Azo Dye in High Glass Transition Temperature Polyimides , 1997 .

[15]  S Kawata,et al.  Reflection confocal microscope readout system for three-dimensional photochromic optical data storage. , 1998, Optics letters.

[16]  Satoshi Kawata,et al.  Individualized optically induced orientation of photochemical isomers , 1999 .