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Side-group switching between metal-to-ligand charge-transfer and metal-centered excited state properties in iron(II) N-heterocyclic carbene complexes

Lindh, Linnea (författare)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,LTH profilområde: Nanovetenskap och halvledarteknologi,LTH profilområden,LU profilområde: Ljus och material,Lunds universitets profilområden,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,LTH Profile Area: Nanoscience and Semiconductor Technology,LTH Profile areas,Faculty of Engineering, LTH,LU Profile Area: Light and Materials,Lund University Profile areas
Rosemann, Nils W. (författare)
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
Losada, Iria Bolaño (författare)
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,LU profilområde: Ljus och material,Lunds universitets profilområden,Other operations, LTH,Faculty of Engineering, LTH,Computational Chemistry,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,LU Profile Area: Light and Materials,Lund University Profile areas
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Persson, Samuel (författare)
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
Goriya, Yogesh (författare)
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
Fan, Hao (författare)
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
Gordivska, Olga (författare)
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
Wärnmark, Kenneth (författare)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,LTH profilområde: Nanovetenskap och halvledarteknologi,LTH profilområden,LU profilområde: Ljus och material,Lunds universitets profilområden,Other operations, LTH,Faculty of Engineering, LTH,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,LTH Profile Area: Nanoscience and Semiconductor Technology,LTH Profile areas,Faculty of Engineering, LTH,LU Profile Area: Light and Materials,Lund University Profile areas
Uhlig, Jens (författare)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,LTH profilområde: Nanovetenskap och halvledarteknologi,LTH profilområden,LTH profilområde: Avancerade ljuskällor,LU profilområde: Ljus och material,Lunds universitets profilområden,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,LTH Profile Area: Nanoscience and Semiconductor Technology,LTH Profile areas,Faculty of Engineering, LTH,LTH Profile Area: Photon Science and Technology,Faculty of Engineering, LTH,LU Profile Area: Light and Materials,Lund University Profile areas
Chábera, Pavel (författare)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,LTH profilområde: Nanovetenskap och halvledarteknologi,LTH profilområden,LTH profilområde: Avancerade ljuskällor,LU profilområde: Ljus och material,Lunds universitets profilområden,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,LTH Profile Area: Nanoscience and Semiconductor Technology,LTH Profile areas,Faculty of Engineering, LTH,LTH Profile Area: Photon Science and Technology,Faculty of Engineering, LTH,LU Profile Area: Light and Materials,Lund University Profile areas
Yartsev, Arkady (författare)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,LTH profilområde: Nanovetenskap och halvledarteknologi,LTH profilområden,LTH profilområde: Avancerade ljuskällor,LU profilområde: Ljus och material,Lunds universitets profilområden,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,LTH Profile Area: Nanoscience and Semiconductor Technology,LTH Profile areas,Faculty of Engineering, LTH,LTH Profile Area: Photon Science and Technology,Faculty of Engineering, LTH,LU Profile Area: Light and Materials,Lund University Profile areas
Persson, Petter (författare)
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,LTH profilområde: Nanovetenskap och halvledarteknologi,LTH profilområden,LU profilområde: Ljus och material,Lunds universitets profilområden,Other operations, LTH,Faculty of Engineering, LTH,Computational Chemistry,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,LTH Profile Area: Nanoscience and Semiconductor Technology,LTH Profile areas,Faculty of Engineering, LTH,LU Profile Area: Light and Materials,Lund University Profile areas
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 (creator_code:org_t)
2024
2024
Engelska.
Ingår i: Coordination Chemistry Reviews. - 0010-8545. ; 506
Relaterad länk:
http://dx.doi.org/10... (free)
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https://lup.lub.lu.s...
https://doi.org/10.1...
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  • Forskningsöversikt (refereegranskat)
Abstract Ämnesord
Stäng  
  • Fe(II) N-heterocyclic carbene (NHC) complexes have emerged over the last decade as a promising class of light-harvesting complexes for a variety of photochemical applications relying on the presence of high-energy excited states of mainly charge-transfer character with excited state lifetimes of tens of picoseconds or longer. Recent spectroscopic investigations have significantly refined the understanding of some of the key prototype complexes of this kind and highlighted the subtle balance between population of triplet metal-to-ligand charge-transfer (3MLCT) and triplet metal-centered (3MC) states as a key issue to better understand and ultimately control the excited state dynamics in these complexes. To present a broader perspective on this issue, we here re-examine and discuss the excited state properties of a series of complexes with different side-groups on a common Fe NHC scaffold. Both the steady-state absorption spectrum and excited state dynamics are influenced by the side-group substitution, and the changes are rationalized based on shifting of the lowest metal-to-ligand charge-transfer (MLCT) state in energy based on the electron-withdrawing or electron-donating properties of the side-groups. Only electron-withdrawing substituents such as carboxylic acid groups ensured that the majority excited population stays in the 3MLCT state for ∼20 ps rather than rapidly converting into metal-centered (MC) states. In other complexes, the 3MLCT state survived <300 fs after which the 3MC state was populated for ∼10 ps. The transient absorption results also show that the dynamics can be switched in a simple manner by deprotonating the carboxylic acid group, which renders some of the complexes pH-sensitive. For the here discussed complexes, the results from transient absorption measurements indicate that the 3MLCT and 3MC states were close enough in energy to enable the side-group to determine the photophysics. The emerging understanding of the 3MLCT-3MC balance, as well as the nature and properties of the 3MC state in these complexes with intermediate ligand field strength is used to provide a broader fundamental perspective required to improve the ligand-design of Fe carbene complexes for issues such as to ensure a long-lived 3MLCT state.

Ämnesord

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)

Nyckelord

Excited state dynamics
Fe(II) N-heterocyclic carbene complexes
Metal-centered states
Metal-to-ligand charge-transfer states
Photophysics and photochemistry of coordination complexes

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