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

J. B. Williams, C. S. Trevisan, M. S. Schöffler, T. Jahnke, I. Bocharova, H. Kim, B. Ulrich, R. Wallauer, F. Sturm, T. N. Rescigno, A. Belkacem, R. Dörner, Th. Weber, C. W. McCurdy, and A. L. Landers

Phys. Rev. Lett. 108, 233002 – Published 8 June 2012

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, ( $H^{+}$ , $H^{+}$ , ${CH}_{2}^{+}$ ). We find the striking result that at low photoelectron energies the molecule is effectively imaged by the focusing of photoelectrons along bond directions.

Received 19 January 2012

DOI:https://doi.org/10.1103/PhysRevLett.108.233002

Authors & Affiliations

J. B. Williams¹, C. S. Trevisan², M. S. Schöffler³, T. Jahnke³, I. Bocharova⁴, H. Kim³, B. Ulrich³, R. Wallauer³, F. Sturm⁴, T. N. Rescigno⁴, A. Belkacem⁴, R. Dörner³, Th. Weber⁴, C. W. McCurdy^4,5, and A. L. Landers¹

¹Department of Physics, Auburn University, Auburn, Alabama 36849, USA
²Department of Sciences and Mathematics, California Maritime Academy, Vallejo, California 94590, USA
³Institut für Kernphysik, J. W. Goethe Universität, Max-von-Laue-Strasse 1, 60438 Frankfurt, Germany
⁴Lawrence Berkeley National Laboratory, Chemical Sciences, Berkeley, California 94720, USA
⁵Department of Chemistry, University of California, Davis, California 95616, USA