Three-pulse photon echo of an excitonic dimer modeled via Redfield theory

被引:31
作者
Kjellberg, P [1 ]
Pullerits, T [1 ]
机构
[1] Lund Univ, Dept Phys Chem, S-22100 Lund, Sweden
关键词
D O I
10.1063/1.2150447
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
In this article the third-order response of an excitonically coupled dimer is studied. The three-pulse photon echo signals were calculated by extracting polarization components from the total polarization in the corresponding phase-matched directions. The total nonlinear response was obtained by numeric propagation of the density matrix, with the exciton-vibrational coupling modeled via Redfield relaxation theory. The full two-dimensional three-pulse photon echo signals and the peak shift were analyzed in terms of the density-matrix dynamics of coherence dephasing and population relaxation. The location of the two-exciton state was found to be essential for proper modeling of the three-pulse photon echo. In particular, an oscillation in the three-pulse photon echo peak shift is found if the two-exciton state is displaced. The oscillations can be related to the dynamics of the one-exciton coherences. (c) 2006 American Institute of Physics.
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页数:9
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