Suchergebnisse

We present an extension of the resolvent-operator method (ROM), originally designed for atomic systems, to extract differential photoelectron spectra (in photoelectron- and nuclear-kinetic energy) for diatomic molecules interacting with strong, ultrashort laser fields in the single active electron approximation. The method is applied to the study of H2+ photodissociation and photoionization by femtosecond laser pulses in the XUV-IR frequency range. In particular, the method is tested (i) in the perturbative regime, for few-photon absorption and bound-bound electronic transitions, and (ii) in the strong-field regime, in which multiphoton absorption and tunneling are present. In the latter case, we show how the differential ROM allows one to track the transition between both regimes. We also analyze isotopic effects by comparing the dynamics of H2+ and D2+ ionization for different pulses. © 2014 American Physical Society. ; This work was accomplished with an allocation of computer time from Mare Nostrum BSC and CCC-UAM and was partially supported by the MICINN Projects No. FIS2010- 15127 and No. CSD 2007-00010, ERA-Chemistry Project No. PIM2010EEC-00751, the European grants No. MC-ITN CORINF and No. MC-RG ATTOTREND, the European COST Action No. CM0702, and European Research Council Advanced Grant No. XCHEM 290853. R.E.F.S. acknowledges a Ph.D. contract from ITN CORINF and Grant No. SFRH/BD/84053/2012 from the Portuguese government. P.R. acknowledges a Juan de la Cierva contract grant from the Spanish MICINN

The role of the nuclear degrees of freedom in nonlinear two-photon single ionization of H2 molecules interacting with short and intense vacuum ultraviolet pulses is investigated, both experimentally and theoretically, by selecting single resonant vibronic intermediate neutral states. This high selectivity relies on the narrow bandwidth and tunability of the pulses generated at the FERMI free-electron laser. A sustained enhancement of dissociative ionization, which even exceeds nondissociative ionization, is observed and controlled as one selects progressively higher vibronic states. With the help of ab initio calculations for increasing pulse durations, the photoelectron and ion energy spectra obtained with velocity map imaging allow us to identify new photoionization pathways. With pulses of the order of 100 fs, the experiment probes a timescale that lies between that of ultrafast dynamical processes and that of steady state excitations ; This research was supported by "Investissements d'Avenir" LabEx PALM (ANR-10-LABX-0039-PALM) and EquipEx ATTOLAB (ANR-11-EQPX-0005- ATTOLAB), as well as by the EU-H2020 Laserlab- Europe 654148. This work is supported by the ERC advanced Grant No. 290853—XCHEM—within the seventh framework program of the European Union. We also acknowledge the financial support from the MINECO Project No. FIS2016-77889-R and the European COST Action XLIC CM1204 and the computer time from the CCC-UAM and Marenostrum Supercomputer. A. P. acknowledges a Ramón y Cajal contract from the Ministerio de Economía y Competitividad (Spain). F. M. acknowledges support from the "Severo Ochoa" Program for Centres of Excellence in R&D (MINECO, Grant No. SEV-2016-0686) and the "María de Maeztu" Program for Units of Excellence in R&D (MDM-2014- 0377). D. D. and M. H. acknowledge support by Institut de Physique (CNRS). M. M. acknowledges support by the Deutsche Forschungsgemeinschaft (DFG) under Grants No. SFB925/A3 and CUI, No. DFG-EXC1074. We gratefully acknowledge the members of the FERMI team at Elettra-Sincrotrone Trieste whose work made this experiment possible