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A low-spin Fe(iii) ...
A low-spin Fe(iii) complex with 100-ps ligand-to-metal charge transfer photoluminescence
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- Chábera, 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,Lund Univ, Dept Chem, Div Phys Chem, Box 124, SE-22100 Lund, Sweden.
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- Liu, Yizhu (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,Lund Univ, Dept Chem, CAS, Box 124, SE-22100 Lund, Sweden.
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- Prakash, Om (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,Lund Univ, Dept Chem, CAS, Box 124, SE-22100 Lund, Sweden.
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- Thyrhaug, Erling (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,Lund Univ, Dept Chem, Div Phys Chem, Box 124, SE-22100 Lund, Sweden.
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- Nahhas, Amal El (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,Lund Univ, Dept Chem, Div Phys Chem, Box 124, SE-22100 Lund, Sweden.
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- Honarfar, Alireza (author)
- Lund University,Lund Univ, Dept Chem, Div Phys Chem, Box 124, SE-22100 Lund, Sweden.
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- Essén, Sofia (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,Lund Univ, Dept Chem, CAS, Box 124, SE-22100 Lund, Sweden.
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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,Lund Univ, Dept Chem, Div Theoret Chem, Box 124, SE-22100 Lund, Sweden.
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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,Lund Univ, Dept Chem, Div Phys Chem, Box 124, SE-22100 Lund, Sweden.;Tech Univ Denmark, Dept Phys, DK-2800 Lyngby, Denmark.
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- Kjær, Kasper S. (author)
- Uppsala universitet,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,Molekylär biomimetik,Biokemi och Strukturbiologi,Centrum för Molekylär Proteinvetenskap,Biochemistry and Structural Biology,Center for Molecular Protein Science,Faculty of Engineering, LTH
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- Handrup, Karsten (author)
- Lund University,Lunds universitet,MAX IV-laboratoriet,MAX IV Laboratory,Lund Univ, Dept Phys, Div Synchrotron Radiat Res, Box 118, SE-22100 Lund, Sweden.
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- Ericson, Fredric (author)
- Uppsala universitet,Mikrosystemteknik,Lund University
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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,Lund Univ, Dept Chem, Div Phys Chem, Box 124, SE-22100 Lund, Sweden.
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- Morgan, Kelsey (author)
- NIST, Boulder, CO 80305 USA.
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- Schnadt, Joachim (author)
- Lund University,Lunds universitet,Synkrotronljusfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Synchrotron Radiation Research,Department of Physics,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Dept Phys, Div Synchrotron Radiat Res, Box 118, SE-22100 Lund, Sweden.
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- Häggström, Lennart (author)
- Uppsala universitet,Materialfysik
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- Ericsson, Tore (author)
- Uppsala universitet,Materialfysik
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- Sobkowiak, Adam (author)
- Uppsala universitet,Strukturkemi
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- Lidin, Sven (author)
- Lund University,Lunds universitet,Naturvetenskapliga fakulteten,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Faculty of Science,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Dept Chem, CAS, Box 124, SE-22100 Lund, Sweden.
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- Huang, Ping (author)
- Uppsala universitet,Lund University,Lunds universitet,Biokemi och Strukturbiologi,Centrum för Molekylär Proteinvetenskap,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Biochemistry and Structural Biology,Center for Molecular Protein Science,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Molekylär biomimetik
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- Styring, Stenbjörn (author)
- Lund University,Lunds universitet,Biokemi och Strukturbiologi,Centrum för Molekylär Proteinvetenskap,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Biochemistry and Structural Biology,Center for Molecular Protein Science,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Dept Chem, Div Phys Chem, Box 124, SE-22100 Lund, Sweden.;Tech Univ Denmark, Dept Phys, DK-2800 Lyngby, Denmark.
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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,Lund Univ, Dept Chem, Div Phys Chem, Box 124, SE-22100 Lund, Sweden.
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- Bendix, Jesper (author)
- Univ Copenhagen, Dept Chem, Univ Pk 5, DK-2100 Copenhagen, Denmark.
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- Lomoth, Reiner (author)
- Uppsala universitet,Fysikalisk kemi
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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,Lund Univ, Dept Chem, Div Phys Chem, Box 124, SE-22100 Lund, Sweden.
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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,Lund Univ, Dept Chem, Div Theoret Chem, Box 124, SE-22100 Lund, Sweden.
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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,Lund Univ, Dept Chem, CAS, Box 124, SE-22100 Lund, Sweden.
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(creator_code:org_t)
- 2017-03-30
- 2017
- English.
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In: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 543:7647, s. 695-699
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Abstract
Subject headings
Close
- Transition-metal complexes are used as photosensitizers1, in light-emitting diodes, for biosensing and in photocatalysis2. A key feature in these applications is excitation from the ground state to a charge-transfer state3,4; the long charge-transfer-state lifetimes typical for complexes of ruthenium5 and other precious metals are often essential to ensure high performance. There is much interest in replacing these scarce elements with Earth-abundant metals, with iron6 and copper7 being particularly attractive owing to their low cost and non-toxicity. But despite the exploration of innovative molecular designs6,8,9,10, it remains a formidable scientific challenge11 to access Earth-abundant transition-metal complexes with long-lived charge-transfer excited states. No known iron complexes are considered12 photoluminescent at room temperature, and their rapid excited-state deactivation precludes their use as photosensitizers13,14,15. Here we present the iron complex [Fe(btz)3]3+ (where btz is 3,3′-dimethyl-1,1′-bis(p-tolyl)-4,4′-bis(1,2,3-triazol-5-ylidene)), and show that the superior σ-donor and π-acceptor electron properties of the ligand stabilize the excited state sufficiently to realize a long charge-transfer lifetime of 100 picoseconds (ps) and room-temperature photoluminescence. This species is a low-spin Fe(iii) d5 complex, and emission occurs from a long-lived doublet ligand-to-metal charge-transfer (2LMCT) state that is rarely seen for transition-metal complexes4,16,17. The absence of intersystem crossing, which often gives rise to large excited-state energy losses in transition-metal complexes, enables the observation of spin-allowed emission directly to the ground state and could be exploited as an increased driving force in photochemical reactions on surfaces. These findings suggest that appropriate design strategies can deliver new iron-based materials for use as light emitters and photosensitizers.
Subject headings
- NATURVETENSKAP -- Kemi -- Teoretisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Theoretical Chemistry (hsv//eng)
- NATURVETENSKAP -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
- NATURAL SCIENCES -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
- NATURVETENSKAP -- Kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences (hsv//eng)
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Chábera, Pavel
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Liu, Yizhu
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Prakash, Om
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Thyrhaug, Erling
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Nahhas, Amal El
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Honarfar, Alirez ...
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show more...
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Essén, Sofia
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Fredin, Lisa A.
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Harlang, Tobias ...
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Kjær, Kasper S.
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Handrup, Karsten
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Ericson, Fredric
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Tatsuno, Hideyuk ...
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Morgan, Kelsey
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Schnadt, Joachim
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Häggström, Lenna ...
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Ericsson, Tore
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Sobkowiak, Adam
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Lidin, Sven
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Huang, Ping
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Styring, Stenbjö ...
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Uhlig, Jens
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Bendix, Jesper
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Lomoth, Reiner
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Sundström, Villy
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Persson, Petter
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Wärnmark, Kennet ...
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