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Title: Chemical bond activation observed with an x-ray laser

Abstract

The concept of bonding and anti-bonding orbitals is fundamental in chemistry. The population of those orbitals and the energetic difference between the two reflect the strength of the bonding interaction. Weakening the bond is expected to reduce this energetic splitting, but the transient character of bond-activation has so far prohibited direct experimental access. Lastly, we apply time-resolved soft X-ray spectroscopy at a free-electron laser to directly observe the decreased bonding–anti-bonding splitting following bond-activation using an ultra short optical laser pulse.

Authors:
 [1];  [2];  [3];  [3];  [4];  [5];  [2];  [6];  [4];  [3];  [6];  [7];  [4];  [3];  [3];  [3];  [3];  [8];  [3];  [3] more »;  [2];  [3];  [9];  [3];  [10];  [11];  [3];  [2];  [12] « less
  1. Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany); SLAC National Accelerator Lab., Menlo Park, CA (United States); Deutsches Elektronen-Synchrotron (DESY) Photon Science, Hamburg (Germany)
  2. Stockholm Univ., Stockholm, (Sweden)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Univ. Hamburg and Center for Free-Electron Laser Science, Hamburg (Germany)
  5. Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany); Univ. Potsdam, Potsdam (Germany)
  6. Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States); Chapman Univ., Orange, CA (United States)
  8. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stockholm Univ., Stockholm, (Sweden)
  9. The Univ. of Liverpool, Liverpool (United Kingdom)
  10. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stockholm Univ., Stockholm, (Sweden); KTH Royal Institute of Technology, Stockholm (Sweden)
  11. Fritz-Haber Institut der Max-Planck-Gesellschaft, Berlin (Germany)
  12. Deutsches Elektronen-Synchrotron (DESY) Photon Science, Hamburg (Germany); Univ. Hamburg and Center for Free-Electron Laser Science, Hamburg (Germany)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1349302
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 7; Journal Issue: 18; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Beye, Martin, Öberg, Henrik, Xin, Hongliang, Dakovski, Georgi L., Dell’Angela, Martina, Föhlisch, Alexander, Gladh, Jörgen, Hantschmann, Markus, Hieke, Florian, Kaya, Sarp, Kühn, Danilo, LaRue, Jerry, Mercurio, Giuseppe, Minitti, Michael P., Mitra, Ankush, Moeller, Stefan P., Ng, May Ling, Nilsson, Anders, Nordlund, Dennis, Nørskov, Jens, Öström, Henrik, Ogasawara, Hirohito, Persson, Mats, Schlotter, William F., Sellberg, Jonas A., Wolf, Martin, Abild-Pedersen, Frank, Pettersson, Lars G. M., and Wurth, Wilfried. Chemical bond activation observed with an x-ray laser. United States: N. p., 2016. Web. doi:10.1021/acs.jpclett.6b01543.
Beye, Martin, Öberg, Henrik, Xin, Hongliang, Dakovski, Georgi L., Dell’Angela, Martina, Föhlisch, Alexander, Gladh, Jörgen, Hantschmann, Markus, Hieke, Florian, Kaya, Sarp, Kühn, Danilo, LaRue, Jerry, Mercurio, Giuseppe, Minitti, Michael P., Mitra, Ankush, Moeller, Stefan P., Ng, May Ling, Nilsson, Anders, Nordlund, Dennis, Nørskov, Jens, Öström, Henrik, Ogasawara, Hirohito, Persson, Mats, Schlotter, William F., Sellberg, Jonas A., Wolf, Martin, Abild-Pedersen, Frank, Pettersson, Lars G. M., & Wurth, Wilfried. Chemical bond activation observed with an x-ray laser. United States. https://doi.org/10.1021/acs.jpclett.6b01543
Beye, Martin, Öberg, Henrik, Xin, Hongliang, Dakovski, Georgi L., Dell’Angela, Martina, Föhlisch, Alexander, Gladh, Jörgen, Hantschmann, Markus, Hieke, Florian, Kaya, Sarp, Kühn, Danilo, LaRue, Jerry, Mercurio, Giuseppe, Minitti, Michael P., Mitra, Ankush, Moeller, Stefan P., Ng, May Ling, Nilsson, Anders, Nordlund, Dennis, Nørskov, Jens, Öström, Henrik, Ogasawara, Hirohito, Persson, Mats, Schlotter, William F., Sellberg, Jonas A., Wolf, Martin, Abild-Pedersen, Frank, Pettersson, Lars G. M., and Wurth, Wilfried. Thu . "Chemical bond activation observed with an x-ray laser". United States. https://doi.org/10.1021/acs.jpclett.6b01543. https://www.osti.gov/servlets/purl/1349302.
@article{osti_1349302,
title = {Chemical bond activation observed with an x-ray laser},
author = {Beye, Martin and Öberg, Henrik and Xin, Hongliang and Dakovski, Georgi L. and Dell’Angela, Martina and Föhlisch, Alexander and Gladh, Jörgen and Hantschmann, Markus and Hieke, Florian and Kaya, Sarp and Kühn, Danilo and LaRue, Jerry and Mercurio, Giuseppe and Minitti, Michael P. and Mitra, Ankush and Moeller, Stefan P. and Ng, May Ling and Nilsson, Anders and Nordlund, Dennis and Nørskov, Jens and Öström, Henrik and Ogasawara, Hirohito and Persson, Mats and Schlotter, William F. and Sellberg, Jonas A. and Wolf, Martin and Abild-Pedersen, Frank and Pettersson, Lars G. M. and Wurth, Wilfried},
abstractNote = {The concept of bonding and anti-bonding orbitals is fundamental in chemistry. The population of those orbitals and the energetic difference between the two reflect the strength of the bonding interaction. Weakening the bond is expected to reduce this energetic splitting, but the transient character of bond-activation has so far prohibited direct experimental access. Lastly, we apply time-resolved soft X-ray spectroscopy at a free-electron laser to directly observe the decreased bonding–anti-bonding splitting following bond-activation using an ultra short optical laser pulse.},
doi = {10.1021/acs.jpclett.6b01543},
journal = {Journal of Physical Chemistry Letters},
number = 18,
volume = 7,
place = {United States},
year = {Thu Sep 01 00:00:00 EDT 2016},
month = {Thu Sep 01 00:00:00 EDT 2016}
}

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Free Publicly Available Full Text
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Citation Metrics:
Cited by: 22 works
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Figures / Tables:

Figure 1 Figure 1: (a): Top: The resonant absorption of an X-ray photon at the oxygen 1$s$ core level probes the unoccupied, antibonding states (green). Bottom: X-ray emission from the core-excited states represents the occupied $p$-density of states, mainly of bonding character.

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