Imaging Polyatomic Molecules in Three Dimensions using Molecular Frame Photoelectron Angular Distributions*

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$^+$, CH$_2^+$]. We find the striking result that at low photoelectron energies the molecule is effectively imaged by the focusing of photoelectrons along bond directions.