Exciton coherence‐size and phonon‐mediated optical nonlinearities in restricted geometries
Exciton coherence‐size and phonon‐mediated optical nonlinearities in restricted geometries
复制标题
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
中科院分区:
文献类型:
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作者:
O. Dubovsky;S. Mukamel
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.
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