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Band-Selective Dynamics in Charge-Transfer Excited Iron Carbene Complexes

Abstract

Ultrafast dynamics of photoinduced charge transfer processes in light-harvesting systems based on Earth-abundant transition metal complexes is of current interest for the development of molecular devices for solar energy conversion applications. A combination of ultrafast spectroscopy and first principles quantum chemical calculations of a recently synthesized iron carbene complex is used to elucidate ultrafast excited state evolution processes in these systems with particular emphasis to investigate the underlying reasons why these complexes show promise in terms of significantly extended lifetimes of charge transfer excited states. Together, our results challenge the traditional excited state landscape for iron-based light harvesting transition metal complexes through radically different ground and excited state properties in alternative oxidation states. This includes intriguing indications of rich band-selective excited state dynamics on ultrafast timescales that are interpreted in terms of excitation energy dependence for excitations into a manifold of charge-transfer states. Some implications of the observed excited state properties and photoinduced dynamics for the utilization of iron carbene complexes for solar energy conversion applications are finally discussed.

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Publication details

The article was received on 07 Dec 2018, accepted on 18 Feb 2019 and first published on 18 Feb 2019


Article type: Paper
DOI: 10.1039/C8FD00232K
Citation: Faraday Discuss., 2019, Accepted Manuscript
  • Open access: Creative Commons BY-NC license
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    Band-Selective Dynamics in Charge-Transfer Excited Iron Carbene Complexes

    P. Chabera, L. A. Fredin, K. S. Kjær, N. W. Rosemann, L. Lind, O. Prakash, Y. Liu, K. Warnmark, J. Uhlig, V. Sundstrom, A. Yartsev and P. Persson, Faraday Discuss., 2019, Accepted Manuscript , DOI: 10.1039/C8FD00232K

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      [Original citation] - Published by The Royal Society of Chemistry.

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