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Manipulating charge...
Manipulating charge transfer excited state relaxation and spin crossover in iron coordination complexes with ligand substitution
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- Zhang, Wenkai (author)
- Stanford Linear Accelerator Center (SLAC)
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- Kjær, Kasper S. (author)
- Lund University,Lunds universitet,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Stanford Linear Accelerator Center (SLAC),Technical University of Denmark
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- Alonso-Mori, Roberto (author)
- Stanford Linear Accelerator Center (SLAC)
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- Bergmann, Uwe (author)
- Stanford Linear Accelerator Center (SLAC)
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- Chollet, Matthieu (author)
- Stanford Linear Accelerator Center (SLAC)
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- Fredin, Lisa A. (author)
- Lund University,Lunds universitet,Beräkningskemi,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Computational Chemistry,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH
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- Hadt, Ryan G. (author)
- Stanford University
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- Hartsock, Robert W. (author)
- Stanford University,Stanford Linear Accelerator Center (SLAC)
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- Harlang, Tobias (author)
- Lund University,Lunds universitet,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH
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- Kroll, Thomas (author)
- Stanford University,Stanford Linear Accelerator Center (SLAC)
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- Kubiček, Katharina (author)
- Max Planck Institute for Biophysical Chemistry
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- Lemke, Henrik T. (author)
- Stanford Linear Accelerator Center (SLAC)
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- Liang, Huiyang W. (author)
- Stanford Linear Accelerator Center (SLAC)
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- Liu, Yizhu (author)
- Lund University,Lunds universitet,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH
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- Nielsen, Martin M. (author)
- Technical University of Denmark
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- Persson, Petter (author)
- Lund University,Lunds universitet,Beräkningskemi,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Computational Chemistry,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH
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- Robinson, Joseph S. (author)
- Stanford Linear Accelerator Center (SLAC)
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- Solomon, Edward I (author)
- Stanford Linear Accelerator Center (SLAC),Stanford University
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- Sun, Zheng (author)
- Stanford Linear Accelerator Center (SLAC)
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- Sokaras, Dimosthenis (author)
- Stanford Linear Accelerator Center (SLAC)
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- van Driel, Tim B (author)
- Technical University of Denmark
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- Weng, Tsu-Chien (author)
- Stanford Linear Accelerator Center (SLAC)
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- Zhu, Diling (author)
- Stanford Linear Accelerator Center (SLAC)
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- Wärnmark, Kenneth (author)
- Lund University,Lunds universitet,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH
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- Sundström, Villy (author)
- Lund University,Lunds universitet,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH
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- Gaffney, Kelly J. (author)
- Stanford Linear Accelerator Center (SLAC)
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(creator_code:org_t)
- 2016
- 2016
- English 9 s.
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In: Chemical Science. - 2041-6520. ; 8:1, s. 515-523
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Abstract
Subject headings
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- Developing light-harvesting and photocatalytic molecules made with iron could provide a cost effective, scalable, and environmentally benign path for solar energy conversion. To date these developments have been limited by the sub-picosecond metal-to-ligand charge transfer (MLCT) electronic excited state lifetime of iron based complexes due to spin crossover-the extremely fast intersystem crossing and internal conversion to high spin metal-centered excited states. We revitalize a 30 year old synthetic strategy for extending the MLCT excited state lifetimes of iron complexes by making mixed ligand iron complexes with four cyanide (CN-;) ligands and one 2,2′-bipyridine (bpy) ligand. This enables MLCT excited state and metal-centered excited state energies to be manipulated with partial independence and provides a path to suppressing spin crossover. We have combined X-ray Free-Electron Laser (XFEL) Kβ hard X-ray fluorescence spectroscopy with femtosecond time-resolved UV-visible absorption spectroscopy to characterize the electronic excited state dynamics initiated by MLCT excitation of [Fe(CN)4(bpy)]2-. The two experimental techniques are highly complementary; the time-resolved UV-visible measurement probes allowed electronic transitions between valence states making it sensitive to ligand-centered electronic states such as MLCT states, whereas the Kβ fluorescence spectroscopy provides a sensitive measure of changes in the Fe spin state characteristic of metal-centered excited states. We conclude that the MLCT excited state of [Fe(CN)4(bpy)]2- decays with roughly a 20 ps lifetime without undergoing spin crossover, exceeding the MLCT excited state lifetime of [Fe(2,2′-bipyridine)3]2+ by more than two orders of magnitude.
Subject headings
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
Publication and Content Type
- art (subject category)
- ref (subject category)
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- By the author/editor
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Zhang, Wenkai
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Kjær, Kasper S.
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Alonso-Mori, Rob ...
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Bergmann, Uwe
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Chollet, Matthie ...
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Fredin, Lisa A.
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show more...
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Hadt, Ryan G.
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Hartsock, Robert ...
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Harlang, Tobias
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Kroll, Thomas
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Kubiček, Kathari ...
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Lemke, Henrik T.
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Liang, Huiyang W ...
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Liu, Yizhu
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Nielsen, Martin ...
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Persson, Petter
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Robinson, Joseph ...
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Solomon, Edward ...
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Sun, Zheng
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Sokaras, Dimosth ...
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van Driel, Tim B
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Weng, Tsu-Chien
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Zhu, Diling
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Wärnmark, Kennet ...
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Sundström, Villy
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Gaffney, Kelly J ...
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- About the subject
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Chemical Science ...
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and Physical Chemist ...
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Chemical Science
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Lund University