Department of Physics and Astronomy, The University of British Columbia, Vancouver, British Columbia V6T 1Z1, Canada.
Department of Chemistry, The University of British Columbia, Vancouver, British Columbia V6T 1Z1, Canada.
J Chem Phys. 2017 Sep 28;147(12):124202. doi: 10.1063/1.5004788.
We use an optical centrifuge to excite coherent rotational wave packets in NO, OCS, and CS molecules with rotational quantum numbers reaching up to J≈465, 690, and 1186, respectively. Time-resolved rotational spectroscopy at such ultra-high levels of rotational excitation can be used as a sensitive tool to probe the molecular potential energy surface at internuclear distances far from their equilibrium values. Significant bond stretching in the centrifuged molecules results in the growing period of the rotational revivals, which are experimentally detected using coherent Raman scattering. We measure the revival period as a function of the centrifuge-induced rotational frequency and compare it with the numerical calculations based on the known Morse-cosine potentials.
我们使用光学离心机在 NO、OCS 和 CS 分子中激发相干转动波包，其转动量子数分别达到约 J≈465、690 和 1186。在如此超高的转动激发水平下进行的时间分辨转动光谱学可以用作探测分子势能面的灵敏工具，探测距离远远超出其平衡值。在被离心的分子中，显著的键拉伸导致转动回复期的增长，这可以通过相干拉曼散射实验来检测。我们测量了回复期作为离心诱导的转动频率的函数，并将其与基于已知的 Morse-cosine 势能的数值计算进行了比较。
