2021, Murillo-Sánchez, Marta L., Reitsma, Geert, Poullain, Sonia Marggi, Fernández-Milán, Pedro, González-Vázquez, Jesús, de Nalda, Rebeca, Martín, Fernando, Vrakking, Marc J. J., Kornilov, Oleg, Bañares, Luis

The time-resolved photodynamics of the methyl iodide cation (CH3I+) are investigated by means of femtosecond XUV-IR pump-probe spectroscopy. A time-delay-compensated XUV monochromator is employed to isolate a specific harmonic, the 9th harmonic of the fundamental 800 nm (13.95 eV, 88.89 nm), which is used as a pump pulse to prepare the cation in several electronic states. A time-delayed IR probe pulse is used to probe the dissociative dynamics on the first excited state potential energy surface. Photoelectrons and photofragment ions - and I+ - are detected by velocity map imaging. The experimental results are complemented with high level ab initio calculations for the potential energy curves of the electronic states of CH3I+ as well as with full dimension on-the-fly trajectory calculations on the first electronically excited state, considering the presence of the IR pulse. The and I+ pump-probe transients reflect the role of the IR pulse in controlling the photodynamics of CH3I+ in the state, mainly through the coupling to the ground state and to the excited state manifold. Oscillatory features are observed and attributed to a vibrational wave packet prepared in the state. The IR probe pulse induces a coupling between electronic states leading to a slow depletion of fragments after the cation is transferred to the ground states and an enhancement of I+ fragments by absorption of IR photons yielding dissociative photoionization. © 2021 The Author(s). Published by IOP Publishing Ltd on behalf of the Institute of Physics and Deutsche Physikalische Gesellschaft.

2020, Wituschek, Andreas, Kornilov, Oleg, Witting, Tobias, Maikowski, Laura, Stienkemeier, Frank, Vrakking, Marc J.J., Bruder, Lukas

The development of schemes for coherent nonlinear time-domain spectroscopy in the extreme-ultraviolet regime (XUV) has so far been impeded by experimental difficulties that arise at these short wavelengths. In this work we present a novel experimental approach, which facilitates the timing control and phase cycling of XUV pulse sequences produced by harmonic generation in rare gases. The method is demonstrated for the generation and high spectral resolution characterization of narrow-bandwidth harmonics (˜14 eV) in argon and krypton. Our technique simultaneously provides high phase stability and a pathway-selective detection scheme for nonlinear signals - both necessary prerequisites for all types of coherent nonlinear spectroscopy. © 2020 The Author(s). Published by IOP Publishing Ltd on behalf of the Institute of Physics and Deutsche Physikalische Gesellschaft.

2018-05-11, Pisanty, Emilio, Hickstein, Daniel D., Galloway, Benjamin R., Durfee, Charles G., Kapteyn, Henry C., Murnane, Margaret M., Ivanov, Misha

The interaction of intense mid-infrared laser fields with atoms and molecules leads to a range of new opportunities, from the production of bright, coherent radiation in the soft x-ray range, to imaging molecular structures and dynamics with attosecond temporal and sub-angstrom spatial resolution. However, all these effects, which rely on laser-driven recollision of an electron removed by the strong laser field and its parent ion, suffer from the rapidly increasing role of the magnetic field component of the driving pulse: the associated Lorentz force pushes the electrons off course in their excursion and suppresses all recollision-based processes, including high harmonic generation as well as elastic and inelastic scattering. Here we show how the use of two non-collinear beams with opposite circular polarizations produces a forwards ellipticity which can be used to monitor, control, and cancel the effect of the Lorentz force. This arrangement can thus be used to re-enable recollision-based phenomena in regimes beyond the long-wavelength breakdown of the dipole approximation, and it can be used to observe this breakdown in high harmonic generation using currently available light sources.

2017-02-02, Torlina, Lisa, Smirnova, Olga

Measuring the time it takes to remove an electron from an atom or molecule during photoionization has been the focus of a number of recent experiments using newly developed attosecond spectroscopies. The interpretation of such measurements, however, depends critically on the measurement protocol and the specific observables available in each experiment. One such protocol relies on high harmonic generation. In this paper, we derive rigorous and general expressions for ionisation and recombination times in high harmonic generation experiments. We show that these times are different from, but related to, ionisation times measured in photoelectron spectroscopy: that is, those obtained using the attosecond streak camera, RABBITT and attoclock methods. We then proceed to use the analytical R-matrix theory to calculate these times and compare them with experimental values.