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Mechanisms universally permitting hyper-Rayleigh scattering

机译:机制普遍允许超瑞利散射

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Hyper-Rayleigh scattering (HRS) is an incoherent variant of second harmonic generation. The theory involves terms of increasing order of optical nonlinearity: for molecules or unit cells that are centrosymmetric, and which accordingly lack even-order susceptibilities, HRS is often regarded as formally forbidden. However, for the three-photon interaction, theory based on the standard electric dipole approximation, represented as El~3, does not include the detail required to describe what is observed experimentally, in the absence of a static field. New results emerge upon extending the theory to include E1~2E2 and E1~2M1, incorporating one electric quadrupolar or magnetic dipolar interaction respectively. Both additional interactions require the deployment of higher orders in the multipole expansion to govern these processes, with the E1~2E2 interaction analogous in rank and parity to a four-wave susceptibility. A key feature of the present work is its foundation upon a formal tensor derivation which does not oversimplify the molecular components, yet leads to results whose interpretation can be correlated with experimental observations. Results are summarized for the perpendicular detection of both parallel and perpendicular polarizations. Using such methods to investigate molecular systems that might have useful nonlinear characteristics, HRS therefore provides a route to data with direct physical interpretation, to enable more sophisticated design of molecules with sought optical properties.
机译:Hyper-Rayleigh散射(HRS)是一种不连贯的第二次谐波产生变体。该理论涉及光学非线性的增加顺序:对于亚离子微分的分子或单位细胞,因此缺乏均衡的敏感性,HRS通常被视为正式禁止。然而,对于三光子相互作用,基于标准电偶极近似的理论表示为EL〜3,不包括在不存在静态场的情况下描述实验观察到的内容所需的细节。在将理论延伸到包括E1〜2E2和E1〜2M1的理论时,分别出现了新的结果,分别包含一个电动四极管或磁性双极相互作用。这两种额外的交互都需要在多极扩展中部署更高的订单来管理这些过程,其中E1〜2E2在等级和奇偶校验中类似于四波易感性的相互作用。本作本作的关键特征是其基础,其在不超薄分子组分的正式张量衍生时,其导致其解释可以与实验观察结果相关的结果。结果总结了平行和垂直偏振的垂直检测。使用这些方法来研究可能具有有用非线性特性的分子系统,因此HRS为具有直接物理解释的数据提供了一种数据,以实现具有寻求光学性质的更复杂的分子设计。

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