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End date: 2024 × DDC: 500 × Has files: Yes × Subject: molecular analysis × Subject: photochemistry ×

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Now showing 1 - 3 of 3
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    Collapse of layer dimerization in the photo-induced hidden state of 1T-TaS2
    ([London] : Nature Publishing Group UK, 2020) Stahl, Quirin; Kusch, Maximilian; Heinsch, Florian; Garbarino, Gaston; Kretzschmar, Norman; Hanff, Kerstin; Rossnagel, Kai; Geck, Jochen; Ritschel, Tobias
    Photo-induced switching between collective quantum states of matter is a fascinating rising field with exciting opportunities for novel technologies. Presently, very intensively studied examples in this regard are nanometer-thick single crystals of the layered material 1T-TaS2, where picosecond laser pulses can trigger a fully reversible insulator-to-metal transition (IMT). This IMT is believed to be connected to the switching between metastable collective quantum states, but the microscopic nature of this so-called hidden quantum state remained largely elusive up to now. Here, we characterize the hidden quantum state of 1T-TaS2 by means of state-of-the-art x-ray diffraction and show that the laser-driven IMT involves a marked rearrangement of the charge and orbital order in the direction perpendicular to the TaS2-layers. More specifically, we identify the collapse of interlayer molecular orbital dimers as a key mechanism for this non-thermal collective transition between two truly long-range ordered electronic crystals.
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    Graphene transistors for real-time monitoring molecular self-assembly dynamics
    (London : Nature Publishing Group, 2020) Gobbi, Marco; Galanti, Agostino; Stoeckel, Marc-Antoine; Zyska, Bjorn; Bonacchi, Sara; Hecht, Stefan; Samorì, Paolo
    Mastering the dynamics of molecular assembly on surfaces enables the engineering of predictable structural motifs to bestow programmable properties upon target substrates. Yet, monitoring self-assembly in real time on technologically relevant interfaces between a substrate and a solution is challenging, due to experimental complexity of disentangling interfacial from bulk phenomena. Here, we show that graphene devices can be used as highly sensitive detectors to read out the dynamics of molecular self-assembly at the solid/liquid interface in-situ. Irradiation of a photochromic molecule is used to trigger the formation of a metastable self-assembled adlayer on graphene and the dynamics of this process are monitored by tracking the current in the device over time. In perspective, the electrical readout in graphene devices is a diagnostic and highly sensitive means to resolve molecular ensemble dynamics occurring down to the nanosecond time scale, thereby providing a practical and powerful tool to investigate molecular self-organization in 2D. © 2020, The Author(s).
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    Few-femtosecond passage of conical intersections in the benzene cation
    ([London] : Nature Publishing Group UK, 2017) Galbraith, M.C.E.; Scheit, S.; Golubev, N.V.; Reitsma, G.; Zhavoronkov, N.; Despré, V.; Lépine, F.; Kuleff, A.I.; Vrakking, M.J.J.; Kornilov, O.; Köppel, H.; Mikosch, J.
    Observing the crucial first few femtoseconds of photochemical reactions requires tools typically not available in the femtochemistry toolkit. Such dynamics are now within reach with the instruments provided by attosecond science. Here, we apply experimental and theoretical methods to assess the ultrafast nonadiabatic vibronic processes in a prototypical complex system - the excited benzene cation. We use few-femtosecond duration extreme ultraviolet and visible/near-infrared laser pulses to prepare and probe excited cationic states and observe two relaxation timescales of 11 ± 3 fs and 110 ± 20 fs. These are interpreted in terms of population transfer via two sequential conical intersections. The experimental results are quantitatively compared with state-of-the-art multi-configuration time-dependent Hartree calculations showing convincing agreement in the timescales. By characterising one of the fastest internal conversion processes studied to date, we enter an extreme regime of ultrafast molecular dynamics, paving the way to tracking and controlling purely electronic dynamics in complex molecules.