Abstract

Rotational dynamics of D2_2 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 D2_2 molecule, determined by Fourier analysis, is the same as Bgas for an isolated D2_2 molecule. Our observations show that the D2_2 molecules inside helium nanodroplets essentially rotate as free D2_2 molecules.

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