ArticleDalton transactions (Cambridge, England : 2003)2021
Molecular light-upconversion: we have had a problem! When excited state absorption (ESA) overcomes energy transfer upconversion (ETU) in Cr(III)/Er(III) complexes.
Article in Dalton transactions (Cambridge, England : 2003), 2021. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 7 papers.
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Who cites it
7 citing papers in PubMed.
- Synthesis of transition metal-sensitized lanthanide near-infrared luminescent nanoparticles.Nature protocols · 2026Review
- Self-assembled multidye-sensitized erbium single molecules for boosting energy transfer light upconversion in solution.Dalton transactions (Cambridge, England : 2003) · 2025Article
- Self-Assembled Tetrahedral [CrInorganic chemistry · 2024Article
- Upconverting photons at the molecular scale with lanthanide complexes.Chemical science · 2024Review
- Recent Progress in Photonic Upconversion Materials for Organic Lanthanide Complexes.Materials (Basel, Switzerland) · 2023Review
- Direct Determination of the Rate of Intersystem Crossing in a Near-IR Luminescent Cr(III) Triazolyl Complex.Journal of the American Chemical Society · 2023Article
- Recyclable optical bioplastics platform for solid state red light harvestingJournal of materials chemistry. A · 2022Article
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Abstract
Nine-coordinate [ErN9] or [ErN3O6] chromophores found in triple helical [Er(L)3]3+ complexes (L corresponds to 2,2',6',2''-terpyridine (tpy), 2,6-(bisbenzimidazol-2-yl)pyridine (bzimpy), 2,6-diethylcarboxypyridine (dpa-ester) or 2,6-diethylcarboxamidopyridine (dpa-diamide) derivatives), [Er(dpa)3]3- (dpa is the 2,6-dipicolinate dianion) and [GaErGa(bpb-bzimpy)3]9+ (bpb-bzimpy is 2,6-bis((pyridin-2-benzimidazol-5-yl)methyl-(benzimidazol-2-yl))pyridine) exhibit NIR (excitation at 801 nm) into visible (emission at 542 nm) linear light upconversion processes in acetonitrile at room temperature. The associated quantum yields 5.5(6) × 10-11 ≤ φuptot(ESA) ≤ 1.7(2) × 10-9 appear to be 1-3 orders of magnitude larger than those predicted by the accepted single-center excited-state absorption mechanism (ESA). Switching to the alternative energy transfer upconversion mechanism (ETU), which operates in multi-centers [CrErCr(bpb-bzimpy)3]9+, leads to an improved quantum yield of φuptot(ETU) = 5.8(6) × 10-8, but also to an even larger discrepancy by 4-6 orders of magnitude when compared with theoretical models. All photophysical studies point to Er(4I13/2) as being the only available 'long-lived' (1.8 ≤ τ ≤ 6.3 μs) and emissive excited state, which works as an intermediate relay for absorbing the second photon, but with an unexpected large cross-section for an intrashell 4f → 4f electronic transition. With this in mind, the ETU mechanism, thought to optimize upconversion via intermetallic Cr → Er communication in [CrErCr(bpb-bzimpy)3]9+, is indeed not crucial and the boosted associated upconversion quantum yield is indebted to the dominant contribution of the single-center erbium ESA process. This curious phenomenon is responsible for the successful implementation of light upconversion in molecular coordination complexes under reasonable light power intensities, which paves the way for applications in medicine and biology. Its origin could be linked with the presence of metal-ligand bonding.
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