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

verfasst von: 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, Stephan Rauschenbach
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.
Externe Organisation(en): Max-Planck-Institut für Festkörperforschung
Imperial College London
Justus-Liebig-Universität Gießen
Technische Universität Braunschweig
University of Oxford
University of Lincoln
École polytechnique fédérale de Lausanne (EPFL)
Typ: Artikel
Journal: Physical review letters
Band: 126
ISSN: 0031-9007
Publikationsdatum: 01.02.2021
Publikationsstatus: Veröffentlicht
Peer-reviewed: Ja
ASJC Scopus Sachgebiete: Physik und Astronomie (insg.)
Elektronische Version(en): https://doi.org/10.1103/PhysRevLett.126.056001 (Zugang: Offen)

BibTeX

@article{bb87fd7a92924726802c45a8407a00cb,
title = "Fast Molecular Compression by a Hyperthermal Collision Gives Bond-Selective Mechanochemistry",
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.",
author = "Lukas Krumbein and Kelvin Anggara and Martina Stella and Tomasz Michnowicz and Hannah Ochner and Sabine Abb and Gordon Rinke and Andr{\'e} Portz and Michael D{\"u}rr and Uta Schlickum and Andrew Baldwin and Andrea Floris and Klaus Kern and Stephan Rauschenbach",
note = "Funding information: Special thanks to Alessandro De Vita, who should have been among the authors. We thank Rico Gutzler, John Polanyi, Claire Vallance, Mark Brouard, Christian Reichardt for fruitful discussions. Calculations were performed on the supercomputers at Max-Planck Computing and Data Facility in Garching. The research is funded by the Max-Planck Society. K. A. thanks Alexander von Humboldt Foundation for financial support. Via our membership of the UK{\textquoteright}s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202, EP/R029431), this work used the ARCHER UK National Supercomputing Service and the UK Materials and Molecular Modelling Hub for computational resources, MMM Hub, which is partially funded by EPSRC (EP/P020194). S. R. designed and supervised the project. S. R., S. A., K. K., and U.S. planned experiments. L. K., S. R., T. M., G. R., and K. A. performed the experiments. L. K., S. R. H. O., K. A., S. A., and A. B. analyzed experimental data. U.S., T. M., A. P., and M. D. performed chemical analysis measurement. K. A., M. S., and A. F. performed the DFT calculations.The authors declare no competing financial interests.",
year = "2021",
month = feb,
day = "1",
doi = "10.1103/PhysRevLett.126.056001",
language = "English",
volume = "126",
journal = "Physical review letters",
issn = "0031-9007",
publisher = "American Physical Society",
number = "5",
}