In extreme ultraviolet spectroscopy, the photoionization process occurring in a molecule due to the absorption of a single photon can trigger an ultrafast nuclear motion in the cation. Taking advantage of attosecond photoelectron interferometry, where the absorption of the extreme ultraviolet photon is accompanied by the exchange of an additional infrared quantum of light, one can investigate the influence of nuclear dynamics by monitoring the characteristics of the photoelectron spectra generated by the two-color field. Here, we show that attosecond photoelectron interferometry is sensitive to the nuclear response by measuring the two-color photoionization spectra in a mixture of methane (CH4) and deuteromethane (CD4). The effect of the different nuclear evolution in the two isotopologues manifests itself in the modification of the amplitude and contrast of the oscillations of the photoelectron peaks. Our work indicates that nuclear dynamics can affect the coherence properties of the electronic wave packet emitted by photoionization on a time scale as short as a few femtoseconds.

Department of Physics Lund University PO Box 118 SE 221 00 Lund Sweden

Institute of Theoretical Physics Faculty of Mathematics and Physics Charles University 5 Holešovǐkách 2 180 00 Prague 8 Czech Republic

Istituto di Fotonica e Nanotecnologie CNR 35131 Padova Italy

Max Born Institute Max Born Str 2A D 12489 Berlin Germany

Max Planck Institut für Kernphysik 69117 Heidelberg Germany

Physikalisches Institut Albert Ludwigs Universität Freiburg Hermann Herder Straße 3 79104 Freiburg Germany

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Anisotropy Parameters for Two-Color Photoionization Phases in Randomly Oriented Molecules: Theory and Experiment in Methane and Deuteromethane