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Abstract Short intense laser pulses are routinely used to induce rotational wave packet dynamics of molecules. Ro-vibrational wave packet dynamics has been explored comparatively infrequently, focusing predominantly on extremely light and rigid molecules such as H ${}_2^{+}$, H₂and D₂. This work presents quantum mechanical calculations that account for the rotationalandthe vibrational degrees of freedom for a heavier and rather floppy diatomic molecule, namely the neon dimer. For pumping by a strong and short non-resonant pump pulse, we identify several phenomena that depend critically on the vibrational (i.e. radial) degree of freedom. Our calculations show (i) fingerprints of the radial dynamics in the alignment signal; (ii) laser-kick induced dissociative dynamics on very short time scales (ejection of highly structured ‘jets’); and (iii) tunneling dynamics that signifies the existence of resonance states, which are supported by the effective potential curves for selected finite relative angular momenta. Our theory predictions can be explored by existing state-of-the-art experiments. 

We use one-photon excitation to promote $K$-shell electrons of formic acid (which has a planar equilibrium structure) to an antibonding ${\pi }^{*}$orbital. The excited molecule is known to have a (chiral) pyramidal equilibrium structure. In our experiment, we determine the handedness of the excited molecule by imaging the momenta of charged fragments, which occur after its Coulomb explosion triggered by Auger-Meitner decay cascades succeeding the excitation. We find that the handedness of the excited molecule depends on its spatial orientation with respect to the propagation (or polarization) direction of the exciting photon. The effect is largely independent of the exact polarization properties of the light driving the $1s\to {\pi }^{*}$excitation. Published by the American Physical Society2024