Third-order optical nonlinearities of sol-gel silica coating films containing J-like aggregates of a cyanine dye, NK-1967

The third-order optical nonlinearities and responses of sol-gel silica coating films containing J-like aggregates of a cyanine dye, NK-1967, were measured by the femtosecond degenerate four-wave mixing (DFWM) technique under resonant conditions. While NK-1967 in aqueous solution showed an absorption maximum at 742 nm, J-like aggregates of NK-1967 in sol-gel silica coating films showed that at 877 nm. Though the sol-gel silica coating films were stable at room temperature, they began to decompose after 10 minute irradiation at a laser power of 5 GW / cm2. The temporal profiles of the DFWM signal were measured with a time resolution of 0.3 ps, and were found to be almost same as that of CCl4, i.e., the coherent instantaneous nonlinear response was dominant. The contribution of slow response with decay time constants of ca. 1 ps was very small. The electronic component of the effective third-order optical nonlinear susceptibility of one of the films had a value of ca. 2.0 x 10-8 esu at 850 nm. The present value for the sol-gel silica coating film containing the J-like aggregates of NK-1967 is four orders of magnitude greater than that of CS2.

[1]  H. Kawashima,et al.  Large χ(3) of squarylium dye J aggregates measured using the Z-scan technique , 2001 .

[2]  E. Walker,et al.  The optical properties of crystalline 1,1′‐diethyl‐2,2′‐cyanine iodide , 1976 .

[3]  R. Gagel,et al.  Evidence for biexcitons and dynamic Stark effect in J-aggregates from femtosecond spectroscopy , 1994 .

[4]  G. Scheibe,et al.  Über die Veränderlichkeit der Absorptionsspektren in Lösungen und die Nebenvalenzen als ihre Ursache , 1937 .

[5]  D. Marquardt.  An Algorithm for Least-Squares Estimation of Nonlinear Parameters , 1963 .

[6]  J. E. Maskasky.  Molecular orientation of individual J aggregates on gelatin-grown AgBr tabular microcrystals , 1991 .

[7]  EDWIN E. JELLEY,et al.  Spectral Absorption and Fluorescence of Dyes in the Molecular State , 1936, Nature.

[8]  Kazuo Kasatani.  Large electronic third-order optical nonlinearities of cyanine dyes measured by resonant femtosecond degenerate four-wave mixing , 2003 .

[9]  K. Misawa,et al.  New fabrication method for highly oriented J aggregates dispersed in polymer films , 1993 .

[10]  D. Wiersma,et al.  Dephasing-induced damping of superradiant emission in J-aggregates , 1990 .

[11]  Y. Yamaguchi,et al.  Local reflection micro-spectroscopy of excitons in fibril-shaped molecular J-aggregates prepared in PVA thin films , 2003 .

[12]  William R. Ware,et al.  Deconvolution of fluorescence decay curves. A critical comparison of techniques , 1979 .

[13]  Koji Ohta,et al.  Femtosecond optical Kerr study of heavy atom effects on the third-order optical nonlinearity of thiophene homologues: purely electronic contribution , 1996 .

[14]  I. Honma,et al.  Synthesis and Nonlinear Optical Susceptibility of Cyanine Dye J-Aggregate Doped Silica Film (I) , 2000 .

[15]  H. Fidder,et al.  A nonlinear optical study of Frenkel excitons in Langmuir—Blodgett films , 1991 .

[16]  K. Yoshihara,et al.  Temperature Dependent Radiative Lifetime of J-Aggregates , 1996 .

[17]  K. Asai,et al.  High nonlinear optical coefficient (χ3=10−7 esu) of cyanine dye J aggregates doped silica film synthesized by a simple sol–gel method , 2002 .

[18]  Kazuo Kasatani,et al.  Large third-order optical nonlinearity and very fast response of cyanine dye doped thin films measured by resonant femtosecond DFWM technique , 2002, SPIE/COS Photonics Asia.

[19]  Kazuo Kasatani,et al.  Resonant third-order optical nonlinearities of thin films containing J-aggregates of a cyanine dye or a squarylium dye , 2005, SPIE/COS Photonics Asia.

[20]  K. Yoshihara,et al.  Temperature dependence of superradiant emission of BIC J-aggregates , 1994 .

[21]  D. Higgins,et al.  Excitonic transitions in J-aggregates probed by near-field scanning optical microscopy , 1995 .

[22]  M. Drobizhev,et al.  Reorientation of transition dipoles during exciton relaxation in J-aggregates probed by flourescence anisotropy , 1996 .

[23]  H. Fidder,et al.  Dynamics of Frenkel excitons in disordered molecular aggregates , 1991 .

[24]  K. Yoshihara,et al.  Two-exciton emission of BIC J-aggregates , 1994 .

[25]  K. Misawa,et al.  Giant static dipole moment change on electronic excitation in highly oriented J-aggregates , 1994 .

[26]  Ray H. Baughman,et al.  Optical Nonlinearities in One-Dimensional-Conjugated Polymer Crystals. , 1976 .

[27]  M. Auweraer,et al.  Relaxation dynamics of excitons in J-aggregates revealing a two-component Davydov splitting , 1998 .