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- ItemDelayed relaxation of highly excited naphthalene cations(Bristol : IOP Publ., 2020) Reitsma, G.; Hummert, J.; Dura, J.; Loriot, V.; Vrakking, M.J.J.; Lépine, F.; Kornilov, O.The efficiency of energy transfer in ultrafast electronic relaxation of molecules depends strongly on the complex interplay between electronic and nuclear motion. In this study we use wavelength-selected XUV pulses to induce relaxation dynamics of highly excited cationic states of naphthalene. Surprisingly, the observed relaxation lifetimes increase with the cationic excitation energy. We propose that this is a manifestation of a quantum mechanical population trapping that leads to delayed relaxation of molecules in the regions with a high density of excited states. © 2019 Published under licence by IOP Publishing Ltd.
- ItemGeneration and characterization of isolated attosecond pulses for coincidence spectroscopy at 100 kHz repetition rate(Bristol : IOP Publ., 2020) Witting, T.; Furch, F.; Osolodkov, M.; Schell, F.; Menoni, C.; Schulz, C.P.; Vrakking, M.J.J.An attosecond pump-probe beamline with 100 kHz repetition rate for coincidence experiments has been developed. It is based on non-collinear optical parametric chirped pulse ampli-cation and delivers 100 µJ sub-4 fs to an high-harmonic generation source. Details on the generation and characterization of isolated attosecond pulses will be presented. © 2019 Published under licence by IOP Publishing Ltd.
- ItemSignatures of Light-Induced Potential Energy Surfaces in H2+(Bristol : IOP Publ., 2020) Kübel, M.; Spanner, M.; Dube, Z.; Naumov, A. Yu; Vrakking, M.J.J.; Corkum, P.B.; Villeneuve, D.M.; Staudte, A.Using theory and Cold Target Recoil Ion Momentum Spectroscopy we find signatures of light-induced molecular potential energy surfaces in the 3-dimensional proton momentum distributions of dissociating H+2. © 2020 Journal of Physics: Conference Series. All rights reserved.
- ItemHighly non-linear ionization of atoms induced by intense high-harmonic pulses(Bristol : IOP Publishing, 2020) Senfftleben, B.; Kretschmar, M.; Hoffmann, A.; Sauppe, M.; Tümmler, J.; Will, I.; Nagy, T.; Vrakking, M.J.J.; Rupp, D.; Schütte, B.Intense extreme-ultraviolet (XUV) pulses enable the investigation of XUV-induced non-linear processes and are a prerequisite for the development of attosecond pump - attosecond probe experiments. While highly non-linear processes in the XUV range have been studied at free-electron lasers (FELs), high-harmonic generation (HHG) has allowed the investigation of low-order non-linear processes. Here we suggest a concept to optimize the HHG intensity, which surprisingly requires a scaling of the experimental parameters that differs substantially from optimizing the HHG pulse energy. As a result, we are able to study highly non-linear processes in the XUV range using a driving laser with a modest (˜ 10 mJ) pulse energy. We demonstrate our approach by ionizing Ar atoms up to Ar5 + , requiring the absorption of at least 10 XUV photons. © 2020 The Author(s). Published by IOP Publishing Ltd
- ItemPropagation-assisted generation of intense few-femtosecond high-harmonic pulses(Bristol : IOP Publishing, 2020) Major, B.; Kretschmar, M.; Ghafur, O.; Hoffmann, A.; Kovács, K.; Varjú, K.; Senfftleben, B.; Tümmler, J.; Will, I.; Nagy, T.; Rupp, D.; Vrakking, M.J.J.; Tosa, V.; Schütte, B.The ongoing development of intense high-harmonic generation (HHG) sources has recently enabled highly non-linear ionization of atoms by the absorption of at least 10 extreme-ultraviolet (XUV) photons within a single atom (Senfftleben et al, arXiv:1911.01375). Here we investigate how the generation of these very intense HHG pulses in our 18-m-long beamline is aided by the reshaping of the fundamental, few-cycle, near-infrared (NIR) driving laser within a 30-cm-long HHG Xe medium. Using an incident NIR intensity that is higher than what is required for phase-matched HHG, signatures of reshaping are found by measuring the NIR blueshift and the fluorescence from the HHG medium along the propagation axis. These results are well reproduced by numerical calculations that show temporal compression of the NIR pulses in the HHG medium. The simulations predict that after refocusing an XUV beam waist radius of 320 nm and a clean attosecond pulse train can be obtained in the focal plane, with an estimated XUV peak intensity of 9 × 1015 W cm-2. Our results show that XUV intensities that were previously only available at large-scale facilities can now be obtained using moderately powerful table-top light sources. © 2020 The Author(s). Published by IOP Publishing Ltd
- ItemAttosecond transient absorption spectroscopy without inversion symmetry(Bristol : IOP Publ., 2020) Drescher, L.; Vrakking, M.J.J.; Mikosch, J.Transient absorption is a very powerful observable in attosecond experiments on atoms, molecules and solids and is frequently used in experiments employing phase-locked few-cycle infrared and XUV laser pulses derived from high harmonic generation. We show numerically and analytically that in non-centrosymmetric systems, such as many polyatomic molecules, which-way interference enabled by the lack of parity conservation leads to new spectral absorption features, which directly reveal the laser electric field. The extension of attosecond transient absorption spectroscopy (ATAS) to such targets hence becomes sensitive to global and local inversion symmetry. We anticipate that ATAS will find new applications in non-centrosymmetric systems, in which the carrier-to-envelope phase of the infrared pulse becomes a relevant parameter and in which the orientation of the sample and the electronic symmetry of the molecule can be addressed. © 2020 The Author(s). Published by IOP Publishing Ltd.