Exciton coherence‐size and phonon‐mediated optical nonlinearities in restricted geometries

Exciton coherence‐size and phonon‐mediated optical nonlinearities in restricted geometries
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受限几何形状中的激子相干尺寸和声子介导的光学非线性

DOI:
10.1063/1.461312
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发表时间:
1991
影响因子:
4.4
通讯作者:
S. Mukamel
S. Mukamel
中科院分区:
化学2区
文献类型:
--
作者:
O. Dubovsky;S. Mukamel

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分子纳米结构的光学非线性的大小由控制光学响应的协作性的特征相干长度决定。推导了描述与双激子变量耦合的光学偏振演化的运动方程,并用于计算一维分子晶体或聚合物的三阶光学响应(χ(3))。我们证明了相干长度是由分子内和分子间(非局域)非线性相互作用决定的,并探讨了局域场近似的局限性。声子介导的激子-激子吸引相互作用可能导致束缚激子对(双激子)的形成。我们展示了在双光子吸收和三次谐波产生中,如何容易地观察到非束缚(双激子)和双激子态的共振。
The magnitude of optical nonlinearities of molecular nanostructures is determined by a characteristic coherence‐length which controls the cooperativity of the optical response. Equations of motion describing the evolution of the optical polarization coupled to two‐exciton variables are derived, and used to calculate the third order optical response (χ(3)) of a one‐dimensional molecular crystal or a polymer. We show that the coherence‐length is determined by the interplay between intramolecular and intermolecular (nonlocal) nonlinearities and explore the limitations of the local‐field approximation. Phonon‐mediated exciton–exciton attractive interaction may result in the formation of bound exciton pairs (biexcitons). We show how unbound (two‐exciton) as well as biexciton states could readily be observed as resonances in two‐photon absorption and third harmonic generation.
S. Matsubara:“4. 体内典型和非典型抗精神病药物对多巴胺 D-1、D-2 和血清素 2 受体的占用。”
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