Nonadiabatic Laser-Induced Alignment Dynamics of Molecules on a Surface

Abstract

We demonstrate that a sodium dimer, Na${}_2$($1^3{\Sigma }_u^{+}$), residing on the surface of a helium nanodroplet, can be set into rotation by a nonresonant 1.0 ps infrared laser pulse. The time-dependent degree of alignment measured, exhibits a periodic, gradually decreasing structure that deviates qualitatively from that expected for gas phase dimers. Comparison to alignment dynamics calculated from the time-dependent rotational Schrödinger equation shows that the deviation is due to the alignment dependent interaction between the dimer and the droplet surface. This interaction confines the dimer to the tangential plane of the droplet surface at the point where it resides and is the reason that the observed alignment dynamics is also well-described by a 2D quantum rotor model.

6 pages, 4 figures

References in corpus (5)

• Calculations of static dipole polarizabilities of alkali dimers. Prospects for alignment of ultracold molecules
• Rotational coherence spectroscopy of molecules in helium nanodroplets: Reconciling the time and the frequency domains
• Wave packet dynamics of potassium dimers attached to helium nanodroplets
• Nonadiabatic Laser-Induced Alignment Dynamics of Molecules on a Surface
• Desorption Dynamics of Rb_2 Molecules off the Surface of Helium Nanodroplets

Cited by in corpus (1)

• Nonadiabatic Laser-Induced Alignment Dynamics of Molecules on a Surface