Coherent third-order spectroscopic probes of molecular chirality

Coherent third-order spectroscopic probes of molecular chirality
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DOI:
10.1063/1.1869495
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发表时间:
2005-04-01
影响因子:
4.4
通讯作者:
Mukamel, S
Mukamel, S
中科院分区:
化学2区
文献类型:
--
作者:
Abramavicius, D;Mukamel, S

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利用玻色激子的非线性激子方程的绿色函数解研究了耦合局域非简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,准粒子的散射提供了光学非线性的机制。在光波矢量的一阶中,我们发现了几个由手征引起的各向同性系综的旋转不变张量分量。在动量空间中计算了无限大周期结构的非局域非线性极化率张量,其中问题的大小减少到激子相互作用半径。对α和3(10)螺旋无限肽进行应用。(C)2005年美国物理学会。
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. (C) 2005 American Institute of Physics.