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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Rotationally resolved optical rotation and circular dichroism effects for symmetric top molecules induced by a resonant circularly polarized pumping optical field
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Rotationally resolved optical rotation and circular dichroism effects for symmetric top molecules induced by a resonant circularly polarized pumping optical field

机译：共振圆偏振泵浦光场引起的对称顶部分子的旋转分辨旋光和圆二色性效应

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摘要

The rotationally resolved laser-induced optical activity including the laser-induced optical rotation ( LIOR) and laser-induced circular dichroism (LICD) effects of an IR probing light pumped by a collinear intense resonant circularly polarized light dependent on the third-order susceptibility due to the pure electric dipole interaction for achiral symmetric top molecules in the gas phase is discussed theoretically. The laser-induced optical activity contains four distinct contributions named A, B, C, and D terms: the B term of the LIOR and LICD arising from the rotational wave function perturbed by the pumping light is deduced using the semiclassical perturbation theory, and the expressions for A, C, and D terms, respectively, due to the ac Stark effect, the Boltzmann statistical redistribution, and the alteration of occupation polability, are obtained from previous results [Zheng, R.-H.; Chen, D.-M.; Wei, W.-M.; He, T.-J.; Liu, F.-C. J. Chem. Phys. 2004, 121, 6835]. The microwave-IR double resonant spectrum is proposed to detect the LIOR and LICD effects. As an example, the LIOR and LICD for the HCF3 molecules in the conditions of 298.15 K and 0.3 Torr when the IR probing light sweeps over the rotational-vibrational transition of the nu(5) and nu(1) modes and the right circularly polarized microwave pumping light with the intensity of 1 kW cm(-2) at the resonant frequency 40.84 GHz are calculated on the basis of the B3LYP/6-311++G** computations. The theoretical results indicate that the B term can be of the same order of magnitude as the A and D terms, and the LIOR and LICD can be measurable in comparison to the rotationally resolved MVCD. The laser-induced optical activity may provide useful new information and form a basis for a different kind of optical activity spectroscopy.
机译：旋转分辨的激光诱导的光学活动，包括由共线强共振圆偏振光泵浦的IR探测光的激光诱导旋光（LIOR）和激光诱导圆二色性（LICD）效应，取决于三阶磁化率理论上讨论了气相中非手性对称顶部分子的纯电偶极相互作用。激光诱导的光学活动包含四个不同的贡献，分别称为A，B，C和D项：利用半经典扰动理论推导由泵浦光扰动的旋转波函数引起的LIOR和LICD的B项。分别从ac Stark效应，玻尔兹曼统计重新分布和职业可控性的变化分别获得了A，C和D项的表达式[Zheng，R.-H .; Chen D.-M .;魏维男;他，T.-J .;刘FC J.化学物理2004，121，6835]。提出了微波-红外双共振谱来检测LIOR和LICD效应。例如，当IR探测光掠过nu（5）和nu（1）模的旋转振动跃迁并且右旋圆偏振时，HCF3分子的LIOR和LICD在298.15 K和0.3 Torr的条件下根据B3LYP / 6-311 ++ G **计算，计算出在共振频率40.84 GHz处具有1 kW cm（-2）强度的微波泵浦光。理论结果表明，B项可以与A项和D项具有相同的数量级，并且LIOR和LICD与旋转分解的MVCD相比可以测量。激光诱导的光学活性可能会提供有用的新信息，并为另一种光学活性光谱学奠定基础。

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