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Measurement and Control of Attosecond Charge Migration


Measurement and Control of Attosecond Charge Migration

P. M. Kraus1, B. Mignolet2, D. Baykusheva1, A. Rupenyan1, L. Horný1, E. F. Penka3, O. I. Tolstikhin4, J. Schneider1, F. Jensen5, L. B. Madsen6, A. D. Bandrauk3, F. Remacle2, H. J. Wörner1*

1Laboratorium für Physikalische Chemie, ETH Zürich, 8093 Zürich, Switzerland

2Department of Chemistry, B6c, Université de Liège, B4000 Liège, Belgium

3Laboratoire de Chimie Théorique, Université de Sherbrooke, Québec, Canada

4Moscow Institute of Physics and Technology, Dolgoprudny 141700, Russia

5Department of Chemistry, Aarhus University, Denmark

6Department of Physics and Astronomy, Aarhus University, Denmark

We advance high-harmonic spectroscopy to resolve molecular charge migration [1] in time and space and simultaneously demonstrate extensive control over the process. A multidimensional approach enables us to reconstruct both quantum amplitudes and phases of spatially oriented molecules [2,3] with a resolution of 70-130 attoseconds and to separately reconstruct field-free (a) and laser-driven charge migration (b,c) using driving lasers centered at 800 nm (b) or 1300 nm (c). Our techniques make charge migration in molecules measurable on the attosecond time scale and open new avenues for laser control of electronic primary processes [4].


[1] L. Cederbaum, J. Zobeley, Chem. Phys. Lett. 307, 205 (1999).

[2] P. M. Kraus, A. Rupenyan, H. J. Wörner, Phys. Rev. Lett. 109, 233903 (2012)

[3] P. M. Kraus, D. Baykusheva, H. J. Wörner, Phys. Rev. Lett. 113, 023001 (2014)

[4] R. Weinkauf, E. W. Schlag, T. J. Martinez, R. D. Levine, J. Phys. Chem. A 101, 7702 (1997)