Catalysis in real time using X-ray lasers

A. Nilsson*, J. LaRue, H. Öberg, H. Ogasawara, M. Dell'Angela, M. Beye, H. Öström, J. Gladh, J. K. Nørskov, W. Wurth, F. Abild-Pedersen, L. G.M. Pettersson

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

We describe how the unique temporal and spectral characteristics of X-ray free-electron lasers (XFEL) can be utilized to follow chemical transformations in heterogeneous catalysis in real time. We highlight the systematic study of CO oxidation on Ru(0 0 0 1), which we initiate either using a femtosecond pulse from an optical laser or by activating only the oxygen atoms using a THz pulse. We find that CO is promoted into an entropy-controlled precursor state prior to desorbing when the surface is heated in the absence of oxygen, whereas in the presence of oxygen, CO desorbs directly into the gas phase. We monitor the activation of atomic oxygen explicitly by the reduced split between bonding and antibonding orbitals as the oxygen comes out of the strongly bound hollow position. Applying these novel XFEL techniques to the full oxidation reaction resulted in the surprising observation of a significant fraction of the reactants at the transition state through the electronic signature of the new bond formation.

Original languageEnglish
JournalChemical Physics Letters
Volume675
Pages (from-to)145-173
Number of pages29
ISSN0009-2614
DOIs
Publication statusPublished - 2017
Externally publishedYes

Cite this

Nilsson, A., LaRue, J., Öberg, H., Ogasawara, H., Dell'Angela, M., Beye, M., ... Pettersson, L. G. M. (2017). Catalysis in real time using X-ray lasers. Chemical Physics Letters, 675, 145-173. https://doi.org/10.1016/j.cplett.2017.02.018
Nilsson, A. ; LaRue, J. ; Öberg, H. ; Ogasawara, H. ; Dell'Angela, M. ; Beye, M. ; Öström, H. ; Gladh, J. ; Nørskov, J. K. ; Wurth, W. ; Abild-Pedersen, F. ; Pettersson, L. G.M. / Catalysis in real time using X-ray lasers. In: Chemical Physics Letters. 2017 ; Vol. 675. pp. 145-173.
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title = "Catalysis in real time using X-ray lasers",
abstract = "We describe how the unique temporal and spectral characteristics of X-ray free-electron lasers (XFEL) can be utilized to follow chemical transformations in heterogeneous catalysis in real time. We highlight the systematic study of CO oxidation on Ru(0 0 0 1), which we initiate either using a femtosecond pulse from an optical laser or by activating only the oxygen atoms using a THz pulse. We find that CO is promoted into an entropy-controlled precursor state prior to desorbing when the surface is heated in the absence of oxygen, whereas in the presence of oxygen, CO desorbs directly into the gas phase. We monitor the activation of atomic oxygen explicitly by the reduced split between bonding and antibonding orbitals as the oxygen comes out of the strongly bound hollow position. Applying these novel XFEL techniques to the full oxidation reaction resulted in the surprising observation of a significant fraction of the reactants at the transition state through the electronic signature of the new bond formation.",
author = "A. Nilsson and J. LaRue and H. {\"O}berg and H. Ogasawara and M. Dell'Angela and M. Beye and H. {\"O}str{\"o}m and J. Gladh and N{\o}rskov, {J. K.} and W. Wurth and F. Abild-Pedersen and Pettersson, {L. G.M.}",
year = "2017",
doi = "10.1016/j.cplett.2017.02.018",
language = "English",
volume = "675",
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journal = "Chemical Physics Letters",
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Nilsson, A, LaRue, J, Öberg, H, Ogasawara, H, Dell'Angela, M, Beye, M, Öström, H, Gladh, J, Nørskov, JK, Wurth, W, Abild-Pedersen, F & Pettersson, LGM 2017, 'Catalysis in real time using X-ray lasers', Chemical Physics Letters, vol. 675, pp. 145-173. https://doi.org/10.1016/j.cplett.2017.02.018

Catalysis in real time using X-ray lasers. / Nilsson, A.; LaRue, J.; Öberg, H.; Ogasawara, H.; Dell'Angela, M.; Beye, M.; Öström, H.; Gladh, J.; Nørskov, J. K.; Wurth, W.; Abild-Pedersen, F.; Pettersson, L. G.M.

In: Chemical Physics Letters, Vol. 675, 2017, p. 145-173.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Catalysis in real time using X-ray lasers

AU - Nilsson, A.

AU - LaRue, J.

AU - Öberg, H.

AU - Ogasawara, H.

AU - Dell'Angela, M.

AU - Beye, M.

AU - Öström, H.

AU - Gladh, J.

AU - Nørskov, J. K.

AU - Wurth, W.

AU - Abild-Pedersen, F.

AU - Pettersson, L. G.M.

PY - 2017

Y1 - 2017

N2 - We describe how the unique temporal and spectral characteristics of X-ray free-electron lasers (XFEL) can be utilized to follow chemical transformations in heterogeneous catalysis in real time. We highlight the systematic study of CO oxidation on Ru(0 0 0 1), which we initiate either using a femtosecond pulse from an optical laser or by activating only the oxygen atoms using a THz pulse. We find that CO is promoted into an entropy-controlled precursor state prior to desorbing when the surface is heated in the absence of oxygen, whereas in the presence of oxygen, CO desorbs directly into the gas phase. We monitor the activation of atomic oxygen explicitly by the reduced split between bonding and antibonding orbitals as the oxygen comes out of the strongly bound hollow position. Applying these novel XFEL techniques to the full oxidation reaction resulted in the surprising observation of a significant fraction of the reactants at the transition state through the electronic signature of the new bond formation.

AB - We describe how the unique temporal and spectral characteristics of X-ray free-electron lasers (XFEL) can be utilized to follow chemical transformations in heterogeneous catalysis in real time. We highlight the systematic study of CO oxidation on Ru(0 0 0 1), which we initiate either using a femtosecond pulse from an optical laser or by activating only the oxygen atoms using a THz pulse. We find that CO is promoted into an entropy-controlled precursor state prior to desorbing when the surface is heated in the absence of oxygen, whereas in the presence of oxygen, CO desorbs directly into the gas phase. We monitor the activation of atomic oxygen explicitly by the reduced split between bonding and antibonding orbitals as the oxygen comes out of the strongly bound hollow position. Applying these novel XFEL techniques to the full oxidation reaction resulted in the surprising observation of a significant fraction of the reactants at the transition state through the electronic signature of the new bond formation.

U2 - 10.1016/j.cplett.2017.02.018

DO - 10.1016/j.cplett.2017.02.018

M3 - Journal article

VL - 675

SP - 145

EP - 173

JO - Chemical Physics Letters

JF - Chemical Physics Letters

SN - 0009-2614

ER -

Nilsson A, LaRue J, Öberg H, Ogasawara H, Dell'Angela M, Beye M et al. Catalysis in real time using X-ray lasers. Chemical Physics Letters. 2017;675:145-173. https://doi.org/10.1016/j.cplett.2017.02.018