Imaging polyatomic molecules in three dimensions using molecular frame photoelectron angular distributions

Phys Rev Lett. 2012 Jun 8;108(23):233002. doi: 10.1103/PhysRevLett.108.233002. Epub 2012 Jun 8.

Abstract

We demonstrate a method for determining the full three-dimensional molecular-frame photoelectron angular distribution in polyatomic molecules using methane as a prototype. Simultaneous double Auger decay and subsequent dissociation allow measurement of the initial momentum vectors of the ionic fragments and the photoelectron in coincidence, allowing full orientation by observing a three-ion decay pathway, (H+, H+, CH2(+)). We find the striking result that at low photoelectron energies the molecule is effectively imaged by the focusing of photoelectrons along bond directions.