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Subject: ultrafast spectroscopy × WGL Institute: MBI ×

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    Attosecond 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.
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    Phase cycling of extreme ultraviolet pulse sequences generated in rare gases
    ([London] : IOP, 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.
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    Non-instantaneous polarization dynamics in dielectric media
    (Berlin : Weierstraß-Institut für Angewandte Analysis und Stochastik, 2014) Hofmann, Michael; Hyyti, Janne; Birkholz, Simon; Bock, Martin; Das, Susanta K.; Grunwald, Rüdiger; Hoffmann, Mathias; Nagy, Tamas; Demircan, Ayhan; Jupé, Marco; Ristau, Detlev; Morgner, Uwe; Brée, Carsten; Woerner, Michael; Elsaesser, Thomas; Steinmeyer, Günter
    Third-order optical nonlinearities play a vital role for generation1,2 and characterization 3-5 of some of the shortest optical pulses to date, for optical switching applications6,7, and for spectroscopy8,9. In many cases, nonlinear optical effects are used far off resonance, and then an instantaneous temporal response is expected. Here, we show for the first time resonant frequency-resolved optical gating measurements1012 that indicate substantial nonlinear polarization relaxation times up to 6.5 fs in dielectric media, i.e., significantly beyond the shortest pulses directly available from commercial lasers. These effects are among the fastest effects observed in ultrafast spectroscopy. Numerical solutions of the time-dependent Schrödinger equation13,14 are in excellent agreement with experimental observations. The simulations indicate that pulse generation and characterization in the ultraviolet may be severely affected by this previously unreported effect. Moreover, our approach opens an avenue for application of frequency-resolved optical gating as a highly selective spectroscopic probe in high-field physics.