Laser-induced rotation of iodine molecules in He-nanodroplets: revivals and breaking-free

Abstract

Rotation of molecules embedded in He nanodroplets is explored by a combination of fs laser-induced alignment experiments and angulon quasiparticle theory. We demonstrate that at low fluence of the fs alignment pulse, the molecule and its solvation shell can be set into coherent collective rotation lasting long enough to form revivals. With increasing fluence, however, the revivals disappear -- instead, rotational dynamics as rapid as for an isolated molecule is observed during the first few picoseconds. Classical calculations trace this phenomenon to transient decoupling of the molecule from its He shell. Our results open novel opportunities for studying non-equilibrium solute-solvent dynamics and quantum thermalization.

6+7 pages; 4+1 figures; 1 table

References in corpus (8)

• Thermalization and its mechanism for generic isolated quantum systems
• Chiral effective field theory and nuclear forces
• Worm Algorithm and Diagrammatic Monte Carlo: A New Approach to Continuous-Space Path Integral Monte Carlo Simulations
• Rotation of quantum impurities in the presence of a many-body environment
• Quasiparticle approach to molecules interacting with quantum solvents
• Rotation of cold molecular ions inside a Bose-Einstein condensate
• Anomalous screening of quantum impurities by a neutral environment
• Angular self-localization of impurities rotating in a bosonic bath

Cited by in corpus (29)

• Quantum control of molecular rotation
• Cold Physics and Chemistry: Collisions, Ionization and Reactions inside Helium Nanodroplets Close to Zero K
• Long-lasting field-free alignment of large molecules inside helium nanodroplets
• Rotational friction and diffusion of quantum rotors
• Emergence of non-abelian magnetic monopoles in a quantum impurity problem
• Charged polarons and molecules in a Bose-Einstein Condensate
• Strongly aligned molecules inside helium droplets in the near-adiabatic regime
• Femtosecond photoexcitation dynamics inside a quantum solvent
• Ultrafast relaxation of photoexcited superfluid He nanodroplets
• Rotational coherence spectroscopy of molecules in helium nanodroplets: Reconciling the time and the frequency domains
• Hyperfine-Structure-Induced Depolarization of Impulsively Aligned ${\mathrm{I}}_2$ Molecules
• Femtosecond rotational dynamics of D${}_2$ molecules in superfluid helium nanodroplets
• Long-lived nuclear coherences inside helium nanodroplets
• Fingerprints of angulon instabilities in the spectra of matrix-isolated molecules
• Diagrammatic Monte Carlo approach to angular momentum in quantum many-particle systems
• Theory of the Rotating Polaron: Spectrum and Self-Localization
• Laser-induced dynamics of molecules with strong nuclear quadrupole coupling
• Nonadiabatic Laser-Induced Alignment Dynamics of Molecules on a Surface
• Diagrammatic approach to orbital quantum impurities interacting with a many-particle environment
• Quantum groups as hidden symmetries of quantum impurities
• Excited rotational states of molecules in a superfluid
• Alignment of the CS${}_2$ Dimer Embedded in Helium Droplets Induced by a Circularly Polarized Laser Pulse
• Quantum dynamics of Rb atoms desorbing off the surface of He nanodroplets
• Intermolecular forces and correlations mediated by a phonon bath
• A simple model for high rotational excitations of molecules in a superfluid
• Energy transfer mechanisms in a dipole chain: From energy equipartition to the formation of breathers
• Quantum criticality and formation of a singular Fermi liquid in the attractive SU(N > 2) Anderson model
• Effect of a magnetic field on molecule-solvent angular momentum transfer
• Environment-limited transfer of angular momentum in Bose liquids