Femtosecond rotational dynamics of D$_2$ molecules in superfluid helium nanodroplets
Junjie Qiang, Lianrong Zhou, Peifen Lu, Kang Lin, Yongzhe Ma, Shengzhe, Pan, Chenxu Lu, Wenyu Jiang, Fenghao Sun, Wenbin Zhang, Hui Li, Xiaochun, Gong, Ilya Sh. Averbukh, Yehiam Prior, Constant A. Schouder, Henrik, Stapelfeldt, Igor N. Cherepanov, Mikhail Lemeshko

TL;DR
This study investigates the femtosecond rotational dynamics of D$_2$ molecules within helium nanodroplets, revealing that they rotate similarly to free molecules with persistent wave packet oscillations.
Contribution
It demonstrates that D$_2$ molecules inside helium nanodroplets exhibit free-rotor behavior, with rotational constants matching those of isolated molecules, using femtosecond pump-probe spectroscopy.
Findings
Oscillations with a 185 fs period indicating rotational wave packets.
Rotational constant BHe matches that of free D$_2$ molecules.
Persistent oscillations over more than 500 periods.
Abstract
Rotational dynamics of D molecules inside helium nanodroplets is induced by a moderately intense femtosecond (fs) pump pulse and measured as a function of time by recording the yield of HeD ions, created through strong-field dissociative ionization with a delayed fs probe pulse. The yield oscillates with a period of 185 fs, reflecting field-free rotational wave packet dynamics, and the oscillation persists for more than 500 periods. Within the experimental uncertainty, the rotational constant BHe of the in-droplet D molecule, determined by Fourier analysis, is the same as Bgas for an isolated D molecule. Our observations show that the D molecules inside helium nanodroplets essentially rotate as free D molecules.
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