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  • Jones, Robert W.University of Huddersfield (author)

Direct Determination of the Rate of Intersystem Crossing in a Near-IR Luminescent Cr(III) Triazolyl Complex

  • Article/chapterEnglish2023

Publisher, publication year, extent ...

  • 2023
  • 12 s.

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  • LIBRIS-ID:oai:lup.lub.lu.se:5a642e93-458b-4228-bf1b-bb6ab768bc5a
  • https://lup.lub.lu.se/record/5a642e93-458b-4228-bf1b-bb6ab768bc5aURI
  • https://doi.org/10.1021/jacs.3c01543DOI

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  • Language:English
  • Summary in:English

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  • Subject category:art swepub-publicationtype
  • Subject category:ref swepub-contenttype

Notes

  • A detailed understanding of the dynamics of photoinduced processes occurring in the electronic excited state is essential in informing the rational design of photoactive transition-metal complexes. Here, the rate of intersystem crossing in a Cr(III)-centered spin-flip emitter is directly determined through the use of ultrafast broadband fluorescence upconversion spectroscopy (FLUPS). In this contribution, we combine 1,2,3-triazole-based ligands with a Cr(III) center and report the solution-stable complex [Cr(btmp)2]3+(btmp = 2,6-bis(4-phenyl-1,2,3-triazol-1-yl-methyl)pyridine) (13+), which displays near-infrared (NIR) luminescence at 760 nm (τ = 13.7 μs, φ = 0.1%) in fluid solution. The excited-state properties of 13+are probed in detail through a combination of ultrafast transient absorption (TA) and femtosecond-to-picosecond FLUPS. Although TA spectroscopy allows us to observe the evolution of phosphorescent excited states within the doublet manifold, more significantly and for the first time for a complex of Cr(III), we utilize FLUPS to capture the short-lived fluorescence from initially populated quartet excited states immediately prior to the intersystem crossing process. The decay of fluorescence from the low-lying 4MC state therefore allows us to assign a value of (823 fs)-1to the rate of intersystem crossing. Importantly, the sensitivity of FLUPS to only luminescent states allows us to disentangle the rate of intersystem crossing from other closely associated excited-state events, something which has not been possible in the spectroscopic studies previously reported for luminescent Cr(III) systems.

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  • Auty, Alexander J.University of Sheffield (author)
  • Wu, GuanzhiUniversity of Sheffield (author)
  • Persson, PetterLund 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(Swepub:lu)chem-ppn (author)
  • Appleby, Martin V.University of Sheffield (author)
  • Chekulaev, DimitriUniversity of Sheffield (author)
  • Rice, Craig R.University of Huddersfield (author)
  • Weinstein, Julia A.University of Sheffield (author)
  • Elliott, Paul I.P.University of Huddersfield (author)
  • Scattergood, Paul A.University of Huddersfield (author)
  • University of HuddersfieldUniversity of Sheffield (creator_code:org_t)

Related titles

  • In:Journal of the American Chemical Society145:22, s. 12081-120920002-7863

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