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We demonstrate a method for determining the full three-dimensional molecular-frame photoelectron\udangular distribution in polyatomic molecules using methane as a prototype. Simultaneous double Auger\uddecay and subsequent dissociation allow measurement of the initial momentum vectors of the ionic\udfragments and the photoelectron in coincidence, allowing full orientation by observing a three-ion decay\udpathway, (H??, H??, CH??\ud2 ). We find the striking result that at low photoelectron energies the molecule is\udeffectively imaged by the focusing of photoelectrons along bond direction

Imaging Polyatomic Molecules in Three Dimensions Using Molecular Frame Photoelectron Angular Distributions