Data from: Controlling population of the molecular rotational state and the alignment theoretically by tailored femtosecond laser pulse

We demonstrate that the population of the molecular rotational state through a stimulated impulsive Raman excitation can be controlled by tailoring the femtosecond laser pulse with a V-style phase modulation. The results show that, by precisely manipulating the modulation parameters, both the odd and even populations of the molecular rotational state can be completely suppressed or reconstructed. Meanwhile, the relative excitation between the odd and even populations can be obtained. Finally, we show that field-free molecular alignment can be controlled due to the modulation of the molecular rotational state populations.我们证明，通过采用V型相位调制（V-style phase modulation）对飞秒激光脉冲（femtosecond laser pulse）进行整形，可调控受激脉冲拉曼激发（stimulated impulsive Raman excitation）过程中的分子转动态布居。研究结果表明，通过精准调控调制参数，能够完全抑制或重构分子转动态布居的奇偶分量；同时，还可获取奇偶布居间的相对激发水平。最终我们证实，通过调控分子转动态布居，可实现无场分子准直（field-free molecular alignment）的操控。