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          Institute: Fritz-Haber-Institut     Collection: Molecular Physics     Display Documents

ID: 476676.0, Fritz-Haber-Institut / Molecular Physics
Photoelectron angular distributions from strong-field ionization of oriented molecules
Authors:Holmegaard, Lotte; Hansen, Jonas L.; Kalhøj, Line; Kragh, Sofie Louise; Stapelfeldt, Henrik; Filsinger, Frank; Küpper, Jochen; Meijer, Gerard; Dimitrovski, Darko; Abu-samha, Mahmoud; Martiny, Christian; Madsen, Lars Bojer
Date of Publication (YYYY-MM-DD):2010-05
Title of Journal:Nature Physics
Journal Abbrev.:Nature Phys.
Start Page:428
End Page:432
Copyright:© 2010 Macmillan Publishers Limited. All rights reserved
Review Status:Peer-review
Audience:Experts Only
Abstract / Description:The combination of photoelectron spectroscopy and ultrafast light sources is on track to set new standards for detailed interrogation of dynamics and reactivity of molecules. A crucial prerequisite for further progress is the ability to not only detect the electron kinetic energy, as done in traditional photoelectron spectroscopy, but also the photoelectron angular distributions (PADs) in the molecular frame. Here carbonylsulfide (OCS) and benzonitrile molecules, fixed in space by combined laser and electrostatic fields, are ionized with intense, circularly polarized, 30 femtosecond laser pulses. For 1-dimensionally oriented OCS the molecular frame PADs exhibit pronounced anisotropies, perpendicular to the fixed permanent dipole moment, that are absent in PADs from randomly oriented molecules. For 3-dimensionally oriented benzonitrile additional striking structures appear due to suppression of electron emission in nodal planes of the fixed electronic orbitals. Our theoretical analysis, relying on tunneling ionization theory, shows that the PADs reflect nodal planes, permanent dipole moments and polarizabilities of both the neutral molecule and its cation. The calculated results are exponentially sensitive to changes in these molecular properties thereby pointing to exciting opportunities for time-resolved probing of valence electrons dynamics by intense circularly polarized pulses. Molecular frame PADs from oriented molecules will prove important in other contexts notably in emerging free-electron-laser studies where localized inner shell electrons are knocked off by x-ray pulses.
External Publication Status:published
Document Type:Article
Communicated by:Gerard Meijer
Affiliations:Fritz-Haber-Institut/Molecular Physics
External Affiliations:Department of Chemistry, Aarhus University, 8000 Aarhus C, Denmark;
Interdisciplinary Nanoscience Center (iNANO), Aarhus University, 8000 Aarhus C, Denmark;
Lundbeck Foundation Theoretical Center for Quantum System Research, Department of Physics and Astronomy, Aarhus University, 8000 Aarhus C, Denmark
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