Robert H. Temperton
Site-Selective Orbital Interactions in an Ultrathin Iron-Carbene Photosensitizer Film
Temperton, Robert H.; Rosemann, Nils W.; Guo, Meiyuan; Johansson, Niclas; Fredin, Lisa A.; Prakash, Om; W�rnmark, Kenneth; Handrup, Karsten; Uhlig, Jens; Schnadt, Joachim; Persson, Petter
Authors
Nils W. Rosemann
Meiyuan Guo
Niclas Johansson
Lisa A. Fredin
Om Prakash
Kenneth W�rnmark
Karsten Handrup
Jens Uhlig
Joachim Schnadt
Petter Persson
Abstract
We present the first experimental study of the frontier orbitals in an ultrathin film of the novel hexa-carbene photosensitizer [Fe(btz)3]3+, where btz is 3,3′-dimethyl-1,1′-bis(p-tolyl)-4,4′-bis(1,2,3-triazol-5-ylidene). Resonant photoelectron spectroscopy (RPES) was used to probe the electronic structure of films where the molecular and oxidative integrities had been confirmed with optical and X-ray spectroscopies. In combination with density functional theory calculations, RPES measurements provided direct and site-selective information about localization and interactions of occupied and unoccupied molecular orbitals. Fe 2p, N 1s, and C 1s measurements selectively probed the metal, carbene, and side-group contributions revealing strong metal–ligand orbital mixing of the frontier orbitals. This helps explain the remarkable photophysical properties of iron-carbenes in terms of unconventional electronic structure properties and favorable metal–ligand bonding interactions—important for the continued development of these type of complexes toward light-harvesting and light-emitting applications.
Citation
Temperton, R. H., Rosemann, N. W., Guo, M., Johansson, N., Fredin, L. A., Prakash, O., …Persson, P. (2020). Site-Selective Orbital Interactions in an Ultrathin Iron-Carbene Photosensitizer Film. Journal of Physical Chemistry A, 124(8), 1603-1609. https://doi.org/10.1021/acs.jpca.0c00803
Journal Article Type | Article |
---|---|
Acceptance Date | Feb 3, 2020 |
Online Publication Date | Feb 3, 2020 |
Publication Date | Feb 27, 2020 |
Deposit Date | Apr 16, 2020 |
Publicly Available Date | Apr 16, 2020 |
Journal | The Journal of Physical Chemistry A |
Print ISSN | 1089-5639 |
Electronic ISSN | 1520-5215 |
Publisher | American Chemical Society |
Peer Reviewed | Peer Reviewed |
Volume | 124 |
Issue | 8 |
Pages | 1603-1609 |
DOI | https://doi.org/10.1021/acs.jpca.0c00803 |
Keywords | Physical and Theoretical Chemistry |
Public URL | https://nottingham-repository.worktribe.com/output/4298508 |
Publisher URL | https://pubs.acs.org/doi/abs/10.1021/acs.jpca.0c00803 |
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Publisher Licence URL
https://creativecommons.org/licenses/by/4.0/
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