Laboratory of Physical Chemistry, ETH Zurich, CH-8093 Zurich, Switzerland.
Phys Chem Chem Phys. 2018 Oct 31;20(42):26837-26845. doi: 10.1039/c8cp05233f.
The term values of rovibrational levels of the GK 1Σ+g and H 1Σ+g states of H2 have been measured with absolute and relative accuracies down to 10-4 cm-1 (≈3 MHz) and 10-6 cm-1 (≈30 kHz), respectively, by measuring transitions to long-lived high-n Rydberg states using single-mode cw laser radiation and a collimated supersonic beam of cold H2 molecules. The term values are compared with those determined in earlier experimental and theoretical investigations and the comparison points at discrepancies and a need for improved theoretical treatments of nonadiabatic, relativistic and radiative corrections for these states. The lifetimes of several low-lying rovibrational levels of the GK, H and I+ 1Πg states have been determined in pump-probe experiments. These lifetimes reveal a significant dependence on the electronic, vibrational and rotational excitation and also deviate from results obtained in earlier experimental and theoretical investigations.
GK 1Σ+g 和 H 1Σ+g 态的 H2 的 rovibrational 能级的项值已经通过使用单模连续激光辐射和冷 H2 分子的准直超音速束测量到长寿命高 n Rydberg 态的跃迁，以达到绝对和相对精度分别为 10-4 cm-1（≈3 MHz）和 10-6 cm-1（≈30 kHz）。这些项值与之前的实验和理论研究中确定的值进行了比较，并指出了差异之处，需要改进这些状态的非绝热、相对论和辐射修正的理论处理。在泵浦探测实验中，已经确定了 GK、H 和 I+1Πg 态的几个低能级 rovibrational 的寿命。这些寿命显示出对电子、振动和旋转激发的显著依赖性，并且与早期的实验和理论研究结果也有所偏离。
