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Electron quantum path interferences in strongly laser-driven aligned molecules and their dependence on the molecular alignment is an essential open problem in strong-field molecular physics. Here, we demonstrate an approach which provides direct access to the observation of these interference processes. The approach is based on the combination of the time-gated-ion-microscopy technique with a pump-probe arrangement used to align the molecules and generate high-order harmonics. By spatially resolving the interference pattern produced by the spatiotemporal overlap of the harmonics emitted by the short and long electron quantum paths, we have succeeded in measuring in situ their phase difference and disclose their dependence on molecular alignment. The findings constitute a vital step towards an understanding of strong-field molecular physics and the development of attosecond spectroscopy approaches without the use of auxiliary atomic references.
We investigate how short and long electron trajectory contributions to high harmonic emission and their interferences give access to intra-molecular dynamics. In the case of unaligned molecules, we show experimental evidences that the long trajectory
We investigate the electron quantum path interference effects during high harmonic generation in atomic gas medium driven by ultrashort chirped laser pulses. To achieve that, we identify and vary the different experimentally relevant control paramete
We study high-order harmonic generation in aligned molecules close to the ionization threshold. Two distinct contributions to the harmonic signal are observed, which show very different responses to molecular alignment and ellipticity of the driving
We show that the dependence of high-order harmonic generation (HHG) on the molecular orientation can be understood within a theoretical treatment that does not involve the strong field of the laser. The results for H_2 show excellent agreement with t
We show that high-order harmonics generated from molecules by intense laser pulses can be expressed as the product of a returning electron wave packet and the photo-recombination cross section (PRCS) where the electron wave packet can be obtained fro