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Orbital mechanism of upright CO activation on Fe(100)
Stockholm University, Faculty of Science, Department of Physics. Yangtze Normal University, China.
Number of Authors: 42019 (English)In: Surface and Interface Analysis, ISSN 0142-2421, E-ISSN 1096-9918, Vol. 51, no 9, p. 914-924Article in journal (Refereed) Published
Abstract [en]

The knowledge of bond activation forms a cornerstone for modern chemistry, wherein symmetry rules of electronic activation lie in the heart of bond activation. However, the question as to how a chemical bond is activated remains elusive. By taking CO activated on Fe(100), herein, we have resolved the long-standing fundamental question; we have found that excitations in the adsorbate feature the bond activation. We essentially have discovered contrasting electronic processes in respective sigma and pi electron systems of the adsorbed CO molecule. The sigma electron system is involved in reversible hidden excitations/deexcitations between two occupied sigma orbitals, whereas the pi electron system is subject to irreversible pi to pi* excitations dispersed along the d-band region, which is coupled to the rotational 2 pi electron couplings depending on the strength of molecule-metal interactions. The sigma excitations pertain to the Pauli repulsion mediated quantum nature with energy and entropy marked by the two energy levels, whereas the pi to pi* excitations fall into a new category of electronic excitations contributing to energy and entropy exchanges in a wide and continuous d-band region. The findings that the internal states of the adsorbate are excited and that fundamental connections between the frontier orbitals and low-lying orbitals are established as the molecule comes to the surface may open up new channels to realize more efficient bond activation and renew our thinking on probing the quantum mechanical nature of bond activation at surfaces with further possible impact on manipulation of orbital activation in femtochemistry and attochemistry.

Place, publisher, year, edition, pages
2019. Vol. 51, no 9, p. 914-924
Keywords [en]
CO activation, CO, Fe(100), orbital mechanism, sigma correlation
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:su:diva-173100DOI: 10.1002/sia.6678ISI: 000479227000003OAI: oai:DiVA.org:su-173100DiVA, id: diva2:1359153
Available from: 2019-10-08 Created: 2019-10-08 Last updated: 2019-10-08Bibliographically approved

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