Measurement and laser control of attosecond charge migration in ionized iodoacetylene.
The ultrafast motion of electrons and holes after light-matter interaction is fundamental to a broad range of chemical and biophysical processes. We advanced high-harmonic spectroscopy to resolve spatially and temporally the migration of an electron hole immediately after ionization of iodoacetylene while simultaneously demonstrating extensive control over the process. A multidimensional approach, based on the measurement and accurate theoretical description of both even and odd harmonic orders, enabled us to reconstruct both quantum amplitudes and phases of the electronic states with a resolution of ~100 attoseconds. We separately reconstructed quasi-field-free and laser-controlled charge migration as a function of the spatial orientation of the molecule and determined the shape of the hole created by ionization. Our technique opens the prospect of laser control over electronic primary processes.
Laboratorium für Physikalische Chemie, ETH Zürich, 8093 Zürich, Switzerland.
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Kraus
Department of Chemistry, Université de Liège, B4000 Liège, Belgium. PULSE Institute and Department of Chemistry, Stanford University, Stanford, CA 94305, USA.
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Mignolet
Laboratorium für Physikalische Chemie, ETH Zürich, 8093 Zürich, Switzerland.
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Baykusheva
Laboratorium für Physikalische Chemie, ETH Zürich, 8093 Zürich, Switzerland.
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Rupenyan
Laboratorium für Physikalische Chemie, ETH Zürich, 8093 Zürich, Switzerland.
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Horný
Laboratoire de Chimie Théorique, Université de Sherbrooke, Sherbrooke, Quebec J1K 2R1, Canada.
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Penka
Laboratorium für Physikalische Chemie, ETH Zürich, 8093 Zürich, Switzerland.
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Grassi
Moscow Institute of Physics and Technology, Dolgoprudny 141700, Russia.
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Tolstikhin
Laboratorium für Physikalische Chemie, ETH Zürich, 8093 Zürich, Switzerland.
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Schneider
Department of Chemistry, Aarhus University, 8000 Aarhus C, Denmark.
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Jensen
Department of Physics and Astronomy, Aarhus University, 8000 Aarhus C, Denmark.
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Madsen
Laboratoire de Chimie Théorique, Université de Sherbrooke, Sherbrooke, Quebec J1K 2R1, Canada.
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Bandrauk
Department of Chemistry, Université de Liège, B4000 Liège, Belgium.
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Remacle
Laboratorium für Physikalische Chemie, ETH Zürich, 8093 Zürich, Switzerland. hwoerner@ethz.ch.
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Wörner