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Solvent control of ...
Solvent control of charge transfer excited state relaxation pathways in [Fe(2,2′-bipyridine)(CN)4]2-
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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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- Kunnus, Kristjan (author)
- Stanford Linear Accelerator Center (SLAC)
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- Harlang, Tobias C.B. (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,Technical University of Denmark
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- Van Driel, Tim B. (author)
- Stanford Linear Accelerator Center (SLAC)
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- Ledbetter, Kathryn (author)
- Stanford Linear Accelerator Center (SLAC)
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- Hartsock, Robert W. (author)
- Stanford Linear Accelerator Center (SLAC)
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- Reinhard, Marco E. (author)
- Stanford Linear Accelerator Center (SLAC)
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- Koroidov, Sergey (author)
- Stanford Linear Accelerator Center (SLAC)
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- Li, Lin (author)
- Stanford Linear Accelerator Center (SLAC)
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- Laursen, Mads G. (author)
- Technical University of Denmark
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- Biasin, Elisa (author)
- Stanford Linear Accelerator Center (SLAC),Technical University of Denmark
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- Hansen, Frederik B. (author)
- Technical University of Denmark
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- Vester, Peter (author)
- Technical University of Denmark
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- Christensen, Morten (author)
- Technical University of Denmark
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- Haldrup, Kristoffer (author)
- Technical University of Denmark
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- Nielsen, Martin M. (author)
- Technical University of Denmark
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- Chabera, Pavel (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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- Liu, Yizhu (author)
- Lund University,Lunds universitet,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Faculty of Engineering, LTH
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- Tatsuno, Hideyuki (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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- Timm, Cornelia (author)
- Lund University
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- Uhlig, Jens (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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- Sundstöm, 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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- Németh, Zoltán (author)
- Hungarian Academy of Sciences
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- Szemes, Dorottya Sárosiné (author)
- Wigner Research Centre for Physics, Hungarian Academy of Sciences
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- Bajnóczi, Éva (author)
- Wigner Research Centre for Physics, Hungarian Academy of Sciences
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- Vankó, György (author)
- Wigner Research Centre for Physics, Hungarian Academy of Sciences
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- Alonso-Mori, Roberto (author)
- Stanford Linear Accelerator Center (SLAC)
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- Glownia, James M. (author)
- Stanford Linear Accelerator Center (SLAC)
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- Nelson, Silke (author)
- Stanford Linear Accelerator Center (SLAC)
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- Sikorski, Marcin (author)
- Stanford Linear Accelerator Center (SLAC)
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- Sokaras, Dimosthenis (author)
- Stanford Linear Accelerator Center (SLAC)
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- Lemke, Henrik T. (author)
- Stanford Linear Accelerator Center (SLAC),Paul Scherrer Institute
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- Canton, Sophie E. (author)
- ELI Attosecond Light Pulse Source (ELI-ALPS),German Electron Synchrotron (DESY)
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- Wärnmark, Kenneth (author)
- Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH
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- Persson, Petter (author)
- Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Beräkningskemi,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Computational Chemistry,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH
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- Cordones, Amy A. (author)
- Stanford Linear Accelerator Center (SLAC)
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- Gaffney, Kelly J. (author)
- Stanford Linear Accelerator Center (SLAC)
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(creator_code:org_t)
- 2018
- 2018
- English 12 s.
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In: Physical Chemistry Chemical Physics. - : Royal Society of Chemistry (RSC). - 1463-9076 .- 1463-9084. ; 20:6, s. 4238-4249
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Abstract
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- The excited state dynamics of solvated [Fe(bpy)(CN)4]2-, where bpy = 2,2′-bipyridine, show significant sensitivity to the solvent Lewis acidity. Using a combination of optical absorption and X-ray emission transient spectroscopies, we have previously shown that the metal to ligand charge transfer (MLCT) excited state of [Fe(bpy)(CN)4]2- has a 19 picosecond lifetime and no discernable contribution from metal centered (MC) states in weak Lewis acid solvents, such as dimethyl sulfoxide and acetonitrile.1,2 In the present work, we use the same combination of spectroscopic techniques to measure the MLCT excited state relaxation dynamics of [Fe(bpy)(CN)4]2- in water, a strong Lewis acid solvent. The charge-transfer excited state is now found to decay in less than 100 femtoseconds, forming a quasi-stable metal centered excited state with a 13 picosecond lifetime. We find that this MC excited state has triplet (3MC) character, unlike other reported six-coordinate Fe(ii)-centered coordination compounds, which form MC quintet (5MC) states. The solvent dependent changes in excited state non-radiative relaxation for [Fe(bpy)(CN)4]2- allows us to infer the influence of the solvent on the electronic structure of the complex. Furthermore, the robust characterization of the dynamics and optical spectral signatures of the isolated 3MC intermediate provides a strong foundation for identifying 3MC intermediates in the electronic excited state relaxation mechanisms of similar Fe-centered systems being developed for solar applications.
Subject headings
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
- NATURVETENSKAP -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
- NATURAL SCIENCES -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)
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- By the author/editor
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Kjær, Kasper S.
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Kunnus, Kristjan
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Harlang, Tobias ...
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Van Driel, Tim B ...
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Ledbetter, Kathr ...
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Hartsock, Robert ...
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show more...
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Reinhard, Marco ...
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Koroidov, Sergey
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Li, Lin
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Laursen, Mads G.
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Biasin, Elisa
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Hansen, Frederik ...
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Vester, Peter
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Christensen, Mor ...
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Haldrup, Kristof ...
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Nielsen, Martin ...
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Chabera, Pavel
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Liu, Yizhu
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Tatsuno, Hideyuk ...
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Timm, Cornelia
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Uhlig, Jens
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Sundstöm, Villy
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Németh, Zoltán
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Szemes, Dorottya ...
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Bajnóczi, Éva
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Vankó, György
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Alonso-Mori, Rob ...
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Glownia, James M ...
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Nelson, Silke
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Sikorski, Marcin
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Sokaras, Dimosth ...
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Lemke, Henrik T.
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Canton, Sophie E ...
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Wärnmark, Kennet ...
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Persson, Petter
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Cordones, Amy A.
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Gaffney, Kelly J ...
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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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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Physical Science ...
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and Atom and Molecul ...
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Lund University