Exciton-scattering mechanism for enhanced nonlinear response of molecular nanostructures.
Exciton-scattering mechanism for enhanced nonlinear response of molecular nanostructures.
复制标题
增强分子纳米结构非线性响应的激子散射机制。
DOI：
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发表时间：
1992
期刊：
影响因子：
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通讯作者：
S. Mukamel
中科院分区：
文献类型：
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作者：
J. Leegwater;S. Mukamel
研究了由任意几何形状的耦合二能级分子组成的分子组装体的非线性光学响应，包括非均匀展宽和激子退相。基于运动方程族的某种封闭性，导出了三阶光学极化率的解析表达式。本文导出了具有激子布居弛豫的小晶粒聚集体的三阶响应的精确表达式，并指出在低弛豫速率下，非线性响应的合作部分在d=1时为Γ -1/2，在对数修正下，在d=2和3时为Γ -1
We study the nonlinear optical response of molecular assemblies consisting of coupled two-level molecules with arbitrary geometry including inhomogeneous broadening and exciton dephasing. An analytical expression for the third-order optical susceptibility is derived based on a certain closure of the equation-of-motion hierarchy. An exact expression for the third-order response of small crystalline aggregates with exciton population relaxation is derived, and used to show that for low relaxation rate Γ the cooperative part of the nonlinear response scales as Γ -1/2 in d=1, and up to logarithmic corrections, as Γ -1 in d=2 and 3