Quantum mechanical model of the upper bounds of the cascading contribution to the second hyperpolarizability
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In this paper, the authors investigated the two-molecule cascaded second hyperpolarizability and showed that it will never exceed the fundamental limit of a single molecule with the same number of electrons as the two molecule system.Abstract:
Microscopic cascading of second-order nonlinearities between two molecules has been proposed to yield an enhanced third-order molecular nonlinear-optical response. In this contribution, we investigate the two-molecule cascaded second hyperpolarizability and show that it will never exceed the fundamental limit of a single molecule with the same number of electrons as the two-molecule system. We show the apparent divergence behavior of the cascading contribution to the second hyperpolarizability vanishes when properly taking into account the intermolecular interactions. Although cascading can never lead to a larger nonlinear-optical response than a single molecule, it provides alternative molecular design configurations for creating materials with large third-order susceptibilities that may be difficult to design into a single molecule.read more
Citations
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Sum rules and scaling in nonlinear optics
TL;DR: In this article, an analysis using sum rules and scaling unifies our understanding of the nonlinear-optical response of a broad class of quantum systems through the scale-invariant intrinsic nonlinearities.
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Theory of Molecular Nonlinear Optics
TL;DR: The theory of molecular nonlinear optics based on the sum-over-state (SOS) model is reviewed in this article, where expressions for the linear (αij) polarizability and nonlinear (βijk, γijkl) molecular hyperpolarizabilities in terms of the properties of the molecular states and the electric dipole transition moments for light-induced transitions between them are derived.
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The Local Field Factor and Microscopic Cascading: A Self-Consistent Method Applied to Confined Systems of Molecules
TL;DR: In this article, a simplified self-consistent method was used to address nonlinear-optical cascading phenomena, which showed added microscopic cascading contributions in high-ordered nonlinear susceptibilities through fifth order.
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Symmetry analysis of Raman scattering mediated by neighboring molecules.
TL;DR: A focus is given here to the newly permitted symmetries, and the results include an extended list of irreducible representations for each point group in which such behavior can arise.
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The local-field factor and microscopic cascading: a self-consistent method applied to confined systems of molecules
TL;DR: In this article, a simplified self-consistent method was used to address nonlinear-optical cascading phenomena, which showed added microscopic cascading contributions in high-ordered nonlinear susceptibilities through fifth order.
References
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The Theory of Intermolecular Forces
TL;DR: In this paper, Cartesian tensors and spherical tensors are used to model the intermolecular potentials in the presence of many-body effects and intermolescular forces.