We present combined theoretical and experimental work investigating the angle-resolved phases of the photoionization process driven by a two-color field consisting of an attosecond pulse train and an infrared pulse in an ensemble of randomly oriented molecules. We derive a general form for the two-color photoelectron (and time-delay) angular distribution valid also in the case of chiral molecules and when relative polarizations of the photons contributing to the attosecond photoelectron interferometer differ. We show a comparison between the experimental data and theoretical predictions in an ensemble of methane and deuteromethane molecules, discussing the effect of nuclear dynamics on the photoionization phases. Finally, we demonstrate that the oscillating component and the phase of the two-color signal can be fitted by using complex asymmetry parameters, in perfect analogy to the atomic case.

Department of Physics Lund University P O Box 118 SE 221 00 Lund Sweden

Department of Physics Stockholm University AlbaNova University Center SE 106 91 Stockholm Sweden

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

Istituto di Fotonica e Nanotecnologie CNR 20129 Milano Italy

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

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

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