光到分子的角动量传递理论

Mikhail Maslov, Georgios M. Koutentakis, Mateja Hrast, Oliver H. Heckl, Mikhail Lemeshko
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引用次数: 0

摘要

我们提出了一种描述结构光(如携带轨道角动量的光)与分子相互作用的理论。我们推导的光物质相互作用哈密顿是通过电场的球形梯度与任何非三维旋转点群粒子的(过渡)电多极矩之间的耦合来表达的。因此,我们的模型可以容纳任意复杂的分子和电场结构,而且可以直接扩展到原子或纳米结构。将这一框架应用于分子振荡光谱学,我们揭示了光的自旋角矩和轨道角矩、分子旋转及其质量中心运动之间角动量交换的一般机制。我们表明,拉盖尔-高斯光束的非零涡度可以强烈增强某些被认为在非螺旋光情况下禁止的振荡转换。我们讨论了在最先进的空间分辨光谱测量中观测这些禁止跃迁的实验要求。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Theory of angular momentum transfer from light to molecules

Theory of angular momentum transfer from light to molecules
We present a theory describing the interaction of structured light, such as light carrying orbital angular momentum, with molecules. The light-matter interaction Hamiltonian we derive is expressed through couplings between spherical gradients of the electric field and the (transition) electric multipole moments of a particle of any nontrivial rotation point group. Our model can therefore accommodate an arbitrary complexity of the molecular and electric field structure, and it can be straightforwardly extended to atoms or nanostructures. Applying this framework to rovibrational spectroscopy of molecules, we uncover the general mechanism of angular momentum exchange between the spin and orbital angular momenta of light, molecular rotation, and its center-of-mass motion. We show that the nonzero vorticity of Laguerre-Gaussian beams can strongly enhance certain rovibrational transitions that are considered forbidden in the case of nonhelical light. We discuss the experimental requirements for the observation of these forbidden transitions in state-of-the-art spatially resolved spectroscopy measurements.
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CiteScore
8.60
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