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- W4320578723 abstract "We investigate the third-order nonlinear-optical susceptibility ${ensuremath{chi}}^{(3)}$ in molecular aggregates and its scaling with aggregate size. The aggregate is modeled as a collection of N-interacting, homogeneously broadened two-level systems, where the interaction includes both the static dipole-dipole coupling and superradiant coupling. Our expression for ${ensuremath{chi}}^{(3)}$, derived using Liouville-space Green-function techniques, contains contributions from excitons as well as biexcitons. The scaling of ${ensuremath{chi}}^{(3)}$ with aggregate size and its dependence on the laser detuning and homogeneous and inhomogeneous dephasing rates are analyzed. ${ensuremath{chi}}^{(3)}$ contains terms that scale as ensuremath{sim}${N}^{2}$ and ensuremath{sim}N(N-1). However, under off-resonant conditions these terms interfere destructively, resulting in a linear ensuremath{sim}N scaling, which is precisely what is expected for N monomers. Detailed calculations of phase-conjugate degenerate four-wave mixing and pump-probe spectroscopy are performed. In the first case we predict the existence of a narrow dephasing-induced resonance superposed on the broader superradiant exciton line shape. Pump-probe spectroscopy shows a series of biexciton absorption lines, some of which are superradiantly broadened." @default.
- W4320578723 created "2023-02-15" @default.
- W4320578723 creator A5061538255 @default.
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- W4320578723 date "1989-11-01" @default.
- W4320578723 modified "2023-10-13" @default.
- W4320578723 title "Nonlinear susceptibilities of molecular aggregates: Enhancement of<mml:math xmlns:mml=http://www.w3.org/1998/Math/MathML display=inline><mml:mrow><mml:msup><mml:mrow><mml:mi>χ</mml:mi></mml:mrow><mml:mrow><mml:mn /><mml:mo>(</mml:mo><mml:mn>3</mml:mn><mml:mo>)</mml:mo><mml:mn /></mml:mrow></mml:msup></mml:mrow></mml:math>by size" @default.
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- W4320578723 doi "https://doi.org/10.1103/physreva.40.5783" @default.
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