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The quantum mechanical motion of electrons and nuclei in systems spatially confined to the molecular dimensions occurs on the sub-femtosecond to the femtosecond timescales respectively. Consequently, the study of ultrafast electronic and, in specific cases, nuclear dynamics requires the availability of light pulses with attosecond (asec) duration and of sufficient intensity to induce two-photon processes, essential for probing the intrinsic system dynamics. The majority of atoms, molecules and solids absorb in the extreme-ultraviolet (XUV) spectral region, in which the synthesis of the required attosecond pulses is feasible. Therefore, the XUV spectral region optimally serves the study of such ultrafast phenomena. Here, we present a detailed review of the first 10-GW class XUV attosecond source based on laser driven high harmonic generation in rare gases. The pulse energy of this source largely exceeds other laser driven attosecond sources and is comparable to the pulse energy of femtosecond Free-Electron-Laser (FEL) XUV sources. The measured pulse duration in the attosecond pulse train is 650 ± 80 asec. The uniqueness of the combined high intensity and short pulse duration of the source is evidenced in non-linear XUV-optics experiments. It further advances the implementation of XUV-pump-XUV-probe experiments and enables the investigation of strong field effects in the XUV spectral region.

We study propagation effects due to the finite speed of light in ionization of extended molecular systems. We present a general quantitative theory of these effects and show under which conditions such effects should appear. The finite speed of light propagation effects are encoded in the non-dipole terms of the time-dependent Shrödinger equation and display themselves in the photoelectron momentum distribution projected on the molecular axis. Our numerical modeling for the $$\hbox {H}_{2}^{+}$$ H 2 + molecular ion and the $$\hbox {Ne}_2$$ Ne 2 dimer shows that the finite light propagation time from one atomic center to another can be accurately determined in a table top laser experiment which is much more readily accessible than the ground breaking synchrotron measurement by Grundmann et al. (Science 370:339, 2020).

[EN] A controversy surrounding the “tunnelling time problem” stems from the seeming inability of quantum mechanics to provide, in the usual way, a definition of the duration a particle is supposed to spend in a given region of space. For this reason, the problem is often approached from an “operational” angle. Typically, one tries to mimic, in a quantum case, an experiment which yields the desired result for a classical particle. One such approach is based on the use of a Larmor clock. We show that the difficulty with applying a non-perturbing Larmor clock in order to “time” a classically forbidden transition arises from the quantum Uncertainty Principle. We also demonstrate that for this reason a Larmor time (in fact, any Larmor time) cannot be interpreted as a physical time interval. We provide a theoretical description of the quantities measured by the clock. Financial support of MCIU, through the grant PGC2018-101355-B-100(MCIU/AEI/FEDER,UE) (DS), and of the Basque Government through Grant No. IT986-16 (DS) is gratefully acknowledged. EA acknowledges the financial support of the Ministerio de Economía y Competitividad (MINECO) of the Spanish Government through BCAM Severo Ochoa accreditation SEV-2017-0718 and PID2019-104927GB-C22 grant. This work was also supported by the BERC 2018e2021 Program and ELKARTEK Programme (KK-2020/00049 and KK-2020/00008) funded by the Basque Government.

We study ultrafast ionization dynamics using orthogonally polarized two-color (OTC) laser pulses involving the resonant "first plus second" ($\omega+2\omega$) scheme. The scheme is illustrated by numerical simulations of the time-dependent Schr\"odinger equation and recording the photoelectron momentum distribution. On the basis of the simulations of this resonant ionization, we identify signatures of the dynamic Autler-Townes effect and dynamic interference, in which their characterization is not possible in spectral domain. Taking advantage of the OTC scheme we show that these dynamical effects, which occur at the same time scale, can be characterized in momentum space by controlling the spatial quantum interference. In particular, we show that with the use of this control scheme, one can tailor the properties of the control pulse to lead to enhancement of the ionization rate through the Autler-Townes effect without affecting the dynamic interference. This enhancement is shown to result from constructive interferences between partial photoelectron waves having opposite-parity, and found to manifest by symmetry-breaking of the momentum distribution. The scenario is investigated for a prototype of a hydrogen atom and is broadly applicable to other systems. Our findings may have applications for photoelectron interferometers to control the electron dynamics in time and space, and for accurate temporal characterization of attosecond pulses., Comment: 12 pages, 6 figures

We theoretically demonstrate the control of the polarization direction of isolated attosecond pulses (IAPs) with inhomogeneous two-color fields synthesized by an 800-nm fundamental pulse and a 2000-nm control pulse having crossed linear polarizations. The results show that by using the temporally and spatially shaped field, the high-order harmonic generation (HHG) process can be efficiently controlled. An ultra-broad supercontinuum ranging from 150th to 400th harmonics which covers the water window region is generated. Such a supercontinuum supports the generation of a 64-as linearly polarized IAP, whose polarization direction is at about 45° with respect to the x axis. Moreover, we analyze the influence of the inhomogeneity parameters and the relative angle of the fundamental and control pulses on the IAP generation. It is shown that the polarization direction of the IAP can rotate in a wide range approximately from 8° to 90° relative to the x axis when the inhomogeneity parameters and the relative angle vary.