Photoinduced molecule formation of spatially separated atoms on helium nanodroplets

TL;DR

This study investigates photoinduced molecule formation on helium nanodroplets, revealing that separated atoms can remain isolated or react upon excitation, with implications for understanding atom interactions in superfluid helium environments.

Contribution

It provides a systematic analysis of atom behavior on helium droplets, showing both isolated atom states and reaction pathways upon electronic excitation, which was previously unexplored.

Findings

Separated Rb and Sr atoms can coexist on a droplet without bonding.

Reaction to form RbSr occurs after electronic excitation.

Ground-state Sr atoms can be at the surface or inside the droplet.

Abstract

Besides the use as cold matrix for spectroscopic studies, superfluid helium droplets have served as a cold environment for the synthesis of molecules and clusters. Since vibrational frequencies of molecules in helium droplets exhibit almost no shift compared to the free molecule values, one could assume the solvated particles move frictionless and undergo a reaction as soon as their paths cross. There have been a few unexplained observations that seemed to indicate cases of two species on one droplet not forming bonds but remaining isolated. In this work, we performed a systematic study of helium droplets doped with one rubidium and one strontium atom showing that besides a reaction to RbSr, there is a probability of finding separated Rb and Sr atoms on one droplet that only react after electronic excitation. Our results further indicate that ground-state Sr atoms can reside at the surface as well as inside the droplet.