Real-time vibrational mode-coupling associated with ultrafast geometrical relaxation in polydiacetylene induced by sub-5-fs pulses

被引:89
作者
Kobayashi, T
Shirakawa, A
Matsuzawa, H
Nakanishi, H
机构
[1] Univ Tokyo, Sch Sci, Dept Phys, Tokyo 1130033, Japan
[2] Tohoku Univ, Inst Chem React Sci, Sendai, Miyagi 9808577, Japan
基金
日本学术振兴会;
关键词
D O I
10.1016/S0009-2614(00)00282-7
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The relaxation time of the free-exciton --> geometrically relaxed 2(1)A(g) state in polydiacetylene is determined as 65-80 fs, depending on the probe energy. The vibrational non-equilibrium in the relaxed 2(1)A(g) state is characterized by the modulations of instantaneous frequencies and amplitudes of C-C and C-C stretching modes with a 145-fs oscillation period. The frequency modulation is anti-phase between the two modes, and the amplitude and frequency are also anti-phase for both modes. These are explained by the coupling of the stretching modes through an in-plane bending mode with 230 cm(-1). This is the first real-time observation of dynamic vibrational mode coupling. (C) 2000 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:385 / 393
页数:9
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