AI 中文总结
本文提出利用分子框架角动量取向实现手性旋转动力学，通过正交偏振脉冲破缺对称性，为区分对映选择性、研究手性光学现象提供新途径。
AI 中文摘要
非手性分子可被制备为手性叠加态。本文提出利用分子框架中的角动量取向实现所需的对称性破缺，无需实验室框架取向即可实现旋转控制。我们从同时打破连续空间旋转对称性和分子点群对称性的要求出发，推导了手性旋转动力学的条件。该条件可通过三个微波脉冲、两个非共振光脉冲结合一个太赫兹脉冲，或三个太赫兹脉冲实现，所有脉冲均具有相互正交的偏振方向，后续动力学可通过光电子圆二色性进行探测。我们的结果为区分结构与动态对映选择性、研究随机取向分子中的时间奇手性光学现象开辟了道路。
英文摘要
Achiral molecules can be prepared in superposition states that are chiral. Here, we propose angular momentum orientation in the molecular frame to achieve the required symmetry breaking, exerting rotational control without the need for laboratory frame orientation. We derive the conditions for chiral rotational dynamics from the requirement to simultaneously break the continuous spatial rotational symmetry and the molecular point group symmetry. This can be achieved by three microwave pulses as well as two non-resonant optical pulses in combination with a THz pulse or three THz pulses, all with mutually orthogonal polarization directions, and the ensuing dynamics can be probed by photoelectron circular dichroism. Our results open the way for distinguishing structural from dynamical enantioselectivity and investigating time-odd chiroptical phenomena in randomly oriented molecules.
Comments8 pages, 3 figures
