One-, two- and three-photon spectroscopy of π-conjugated dendrimers:: cooperative enhancement and coherent domains

被引:90
作者
Drobizhev, M
Rebane, A [1 ]
Suo, Z
Spangler, CW
机构
[1] Montana State Univ, Dept Phys, Bozeman, MT 59717 USA
[2] Lebedev Phys Inst, Moscow 119991, Russia
[3] Montana State Univ, Dept Chem & Biochem, Bozeman, MT 59717 USA
关键词
D O I
10.1016/j.jlumin.2004.10.009
中图分类号
O43 [光学];
学科分类号
070207 ; 0803 ;
摘要
We use wavelength tunable femtosecond pulses to measure intrinsic (simultaneous) two-photon absorption (2PA) and three-photon absorption (3PA) molecular cross section in two series of pi-conjugated dendrimers built of identical 4,4'-bis(diphenylamino) stilbene (BDPAS) and 4,4'-bis(diphenylamino) distyrylbenzene (BDPADSB) repeat units. Record large 2PA cross sections, sigma(2) = 10(-46) cm(4) s are obtained for the largest second-generation BDPAS-based dendrimer, as well as zeroth-generation 4-arm BDPADSB-based dendrimer. In both series, maximum 2PA cross section increases nonlinearly with the number of pi-electrons, whereas for higher generations this dependence turns to linear one. 3PA cross section also increases nonlinearly with the size of the system in the series of BDPAS-based molecules, amounting a record large value, sigma(3) 10(-79)cm(6) s(2), for the largest, second-generation dendrimer. We interpret these results in terms of direct inter-branch conjugation, which facilitates cooperative enhancement of the nonlinear-optical response. We propose a simple model which allows us to determine the effective size of coherent domains (extent of conjugation), which, in turn, determines the optimum dendrimer size for most efficient nonlinear response. (c) 2004 Elsevier B.V. All rights reserved.
引用
收藏
页码:291 / 305
页数:15
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