2017, Argenti, L., Jiménez Galán, Á., Taïeb, R., Caillat, J., Maquet, A., Martín, F.

Synopsis In contrast to one-photon transitions and non-resonant multiphoton transitions, time delay in resonant multi-photon electron emission can exhibit large positive and negative values that have no scattering equivalent, due to the interference of multiple ionization paths.

2016, Silva, R.E.F., Rivière, P., Morales, F., Smirnova, O., Ivanov, M., Martín, F.

Isotropic gases irradiated by long pulses of intense IR light can generate very high harmonics of the incident field. It is generally accepted that, due to the symmetry of the generating medium, be it an atomic or an isotropic molecular gas, only odd harmonics of the driving field can be produced. Here we show how the interplay of electronic and nuclear dynamics can lead to a marked breakdown of this standard picture: a substantial part of the harmonic spectrum can consist of even rather than odd harmonics. We demonstrate the effect using ab-initio solutions of the time-dependent Schrödinger equation for and its isotopes in full dimensionality. By means of a simple analytical model, we identify its physical origin, which is the appearance of a permanent dipole moment in dissociating homonuclear molecules, caused by light-induced localization of the electric charge during dissociation. The effect arises for sufficiently long laser pulses and the region of the spectrum where even harmonics are produced is controlled by pulse duration. Our results (i) show how the interplay of femtosecond nuclear and attosecond electronic dynamics, which affects the charge flow inside the dissociating molecule, is reflected in the nonlinear response, and (ii) force one to augment standard selection rules found in nonlinear optics textbooks by considering light-induced modifications of the medium during the generation process.

2015, Trabattoni, A., Klinker, M., González-Vázquez, J., Liu, C., Sansone, G., Linguerri, R., Hochlaf, M., Klei, J., Vrakking, M. J. J., Martín, F., Nisoli, M., Calegari, F.

Studying the interaction of molecular nitrogen with extreme ultraviolet (XUV) radiation is of prime importance to understand radiation-induced processes occurring in Earth’s upper atmosphere. In particular, photoinduced dissociation dynamics involving excited states of N2+ leads to N and N+ atomic species that are relevant in atmospheric photochemical processes. However, tracking the relaxation dynamics of highly excited states of N2+ is difficult to achieve, and its theoretical modeling is notoriously complex. Here, we report on an experimental and theoretical investigation of the dissociation dynamics of N2+ induced by isolated attosecond XUV pulses in combination with few-optical-cycle near-infrared/visible (NIR/VIS) pulses. The momentum distribution of the produced N+ fragments is measured as a function of pump-probe delay with subfemtosecond resolution using a velocity map imaging spectrometer. The time-dependent measurements reveal the presence of NIR/VIS-induced transitions between N2+ states together with an interference pattern that carries the signature of the potential energy curves activated by the XUV pulse. We show that the subfemtosecond characterization of the interference pattern is essential for a semiquantitative determination of the repulsive part of these curves.

2018-01-23, Busto, D., Barreau, L., Isinger, M., Turconi, M., Alexandridi, C., Harth, A., Zhong, S., Squibb, R.J., Kroon, D., Plogmaker, S., Miranda, M., Jiménez-Galán, Á., Argenti, L., Arnold, C.L., Feifel, R., Martín, F., Gisselbrecht, M., L’Huillier, A., Salières, P.

Autoionization, which results from the interference between direct photoionization and photoexcitation to a discrete state decaying to the continuum by configuration interaction, is a well known example of the important role of electron correlation in light–matter interaction. Information on this process can be obtained by studying the spectral, or equivalently, temporal complex amplitude of the ionized electron wave packet. Using an energy-resolved interferometric technique, we measure the spectral amplitude and phase of autoionized wave packets emitted via the sp2+ and sp3+ resonances in helium. These measurements allow us to reconstruct the corresponding temporal profiles by Fourier transform. In addition, applying various time–frequency representations, we observe the build-up of the wave packets in the continuum, monitor the instantaneous frequencies emitted at any time and disentangle the dynamics of the direct and resonant ionization channels.