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Fast Molecular Compression by a Hyperthermal Collision Gives Bond-Selective Mechanochemistry

Lukas Krumbein, Kelvin Anggara, Martina Stella, Tomasz Michnowicz, Hannah Ochner, Sabine Abb, Gordon Rinke, André Portz, Michael Dürr, Uta Schlickum, Andrew Baldwin, Andrea Floris, Klaus Kern, and Stephan Rauschenbach
Phys. Rev. Lett. 126, 056001 – Published 1 February 2021
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Abstract

Using electrospray ion beam deposition, we collide the complex molecule Reichardt’s dye (C41H30NO+) at low, hyperthermal translational energy (2–50 eV) with a Cu(100) surface and image the outcome at single-molecule level by scanning tunneling microscopy. We observe bond-selective reaction induced by the translational kinetic energy. The collision impulse compresses the molecule and bends specific bonds, prompting them to react selectively. This dynamics drives the system to seek thermally inaccessible reactive pathways, since the compression timescale (subpicosecond) is much shorter than the thermalization timescale (nanosecond), thereby yielding reaction products that are unobtainable thermally.

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  • Received 14 July 2020
  • Accepted 7 December 2020

DOI:https://doi.org/10.1103/PhysRevLett.126.056001

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI. Open access publication funded by the Max Planck Society.

Published by the American Physical Society

Physics Subject Headings (PhySH)

Interdisciplinary PhysicsAtomic, Molecular & OpticalCondensed Matter, Materials & Applied Physics

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Selective Bond Breaking with Splat Chemistry

Published 1 February 2021

Colliding a large organic molecule with a surface can break a specific chemical bond in the molecule with surprising precision.

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Authors & Affiliations

Lukas Krumbein1,†, Kelvin Anggara1,†, Martina Stella2, Tomasz Michnowicz1, Hannah Ochner1, Sabine Abb1, Gordon Rinke1, André Portz3, Michael Dürr3, Uta Schlickum1,4, Andrew Baldwin5, Andrea Floris6, Klaus Kern1,7, and Stephan Rauschenbach1,5,*

  • 1Max-Planck-Institut für Festkörperforschung, Heisenbergstrasse 1, DE-70569 Stuttgart, Germany
  • 2Department of Materials, Royal School of Mines, Imperial College London, Exhibition Road, London SW7 2A2, United Kingdom
  • 3Institut für Angewandte Physik, Justus-Liebig-Universität Giessen, Heinrich-Buff-Ring 16, DE-35392 Giessen, Germany
  • 4Institut für Angewandte Physik, Technische Universität Braunschweig, Mendelssohnstrasse 2, DE-38106 Braunschweig, Germany
  • 5Department of Chemistry, Chemistry Research Laboratory, University of Oxford, 12 Mansfield Road, Oxford OX1 3TA, United Kingdom
  • 6School of Chemistry, University of Lincoln, Brayford Pool, Lincoln LN6 7TS, United Kingdom
  • 7Institut de Physique, École Polytechnique Fédérale de Lausanne, Laussane CH-1015, Switzerland

  • *Corresponding Author. stephan.rauschenbach@chem.ox.ac.uk
  • L. K. and K. A. contributed equally to this work.

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Vol. 126, Iss. 5 — 5 February 2021

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