Multidimensional femtosecond spectroscopies of molecular aggregates and semiconductor nanostructures: The nonlinear exciton equations
Multidimensional femtosecond spectroscopies of molecular aggregates and semiconductor nanostructures: The nonlinear exciton equations
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DOI：
10.1063/1.477621
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发表时间：
1998-12-01
影响因子：
4.4
通讯作者：
Mukamel, S
中科院分区：
文献类型：
--
作者：
Chernyak, V;Zhang, WM;Mukamel, S
利用非线性激子方程（NEE）建立了分子聚集体（从Frenkel-Heitler-London哈密顿量开始）和半导体（从两波段模型开始）的非线性光学光谱的统一描述。这些方程明确地遵循与三阶响应相关的一、二、三点动态激子变量的完整集合。在激子-声子耦合中，通过微扰计算的弛豫超算符将核运动的影响纳入其中。利用基于三点松弛核分解的截断方案求解NEE，得到了三阶响应的格林函数表达式。这些结果为设计激子的多维光谱并利用相干转移途径对其进行分析奠定了基础。(C) 1998美国物理研究所。[s0021 - 9606(98) 70545 - 8]。
A unified description of nonlinear optical spectroscopies of molecular aggregates (starting with the Frenkel-Heitler-London Hamiltonian) and semiconductors (starting with the two-band model) is developed using the nonlinear exciton equations (NEE). The equations follow explicitly the complete set of one-, two-, and three-point dynamical exciton variables relevant for the third-order response. Effects of nuclear motions are incorporated through relaxation superoperators calculated perturbatively in exciton-phonon coupling. A Green's function expression for the third-order response is derived by solving the NEE using a new truncation scheme based on factorizing the three-point relaxation kernels. These results set the stage for designing multidimensional spectroscopies of excitons and analyzing them using coherence-transfer pathways. (C) 1998 American Institute of Physics. [S0021-9606(98)70545-8].