ATOMS, SPECTRA, RADIATIONS

Third-harmonic and sum-frequency generation in a quadratically nonlinear polymer by time-ordered ultrashort laser pulses

S. O. Konorov^a, A. A. Ivanov^b, D. A. Akimov^a, A. V. Yakimanskii^c, M. V. Alfimov^b, A. M. Zheltikov<sup>ad

a</sup> M. V. Lomonosov Moscow State University, Faculty of Physics
^b Photochemistry Centre, Russian Academy of Sciences
^c Institute of Macromolecular Compounds RAS, St. Petersburg
^d International Laser Center of Moscow State University

Abstract: Third-harmonic and sum-frequency generation in quadratically nonlinear azopolymer films is experimentally studied using femtosecond chromium forsterite laser pulses. A noncollinear geometry of sum-frequency and third-harmonic generation developed and implemented in this work allows the influence of the time ordering of ultrashort laser pump pulses on nonlinear-optical phenomena to be experimentally observed. Femtosecond laser pulses induce transitions of azopolymer molecules to an electronically excited state and produce vibrational wave packets, leading to an asymmetry in the dependence of the efficiency of second-and third-order nonlinear-optical processes on the delay time between the pump pulses.

PACS: 42.65.-k

Received: 23.06.2004

 English version: Journal of Experimental and Theoretical Physics Letters, 2004, 80:3, 167–171

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