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Coherent third-order spectroscopic probes of molecular chirality

机译:分子手性的相干三阶光谱探针

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摘要

The third-order optical response of a system of coupled localized anharmonic vibrations is studied using a Green's function solution of the nonlinear exciton equations for bosonized excitons,which are treated as interacting quasiparticles.The explicit calculation of two-exciton states is avoided and the scattering of quasiparticles provides the mechanism of optical nonlinearities.To first-order in the optical wave vector we find several rotationally invariant tensor components for isotropic ensembles which are induced by chirality.The nonlocal nonlinear susceptibility tensor is calculated for infinitely large periodic structures in momentum space,where the problem size reduces to the exciton interaction radius.Applications are made to alpha and 3_(10) helical infinite peptides.
机译:利用非线性激子方程的格林函数解(被视为相互作用的准粒子),研究了耦合的局部非谐振动系统的三阶光学响应,避免了两个激子态的显式计算并消除了散射准粒子的分布提供了光学非线性的机制。在光波向量中一阶,我们发现了由手性引起的各向同性集合的几个旋转不变张量分量。计算了动量空间中无限大周期结构的非局部非线性磁化张量,问题大小减小到激子相互作用半径。应用于α和3_(10)螺旋无限肽。

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