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Light-Harvesting and Ultrafast Energy Migration in Porphyrin-Based Metal-Organic Frameworks

Light-Harvesting and Ultrafast Energy Migration in Porphyrin-Based Metal-Organic Frameworks
Son, Ho-JinJin, ShengyePatwardhan, SameerWezenberg, Sander J.Jeong, Nak CheonSo, MonicaWilmer, Christopher E.Sarjeant, Amy A.Schatz, George C.Snurr, Randall Q.Farha, Omar K.Wiederrecht, Gary P.Hupp, Joseph T.
DGIST Authors
Jeong, Nak Cheon
Issue Date
Journal of the American Chemical Society, 135(2), 862-869
Article Type
[5,15 Bis[4 (Pyridyl)Ethynyl] 10,20 Diphenylporphinato]Zinc (ii)[5,15 Dipyridyl 10,20 Bis(Pentafluorophenyl)Porphinato]Zinc (ii)AbsorptionAbsorption IntensityAcetyleneAcetylene DerivativeAddition ReactionAnisotropyAntennaCalculationChlorophyllConjugationControlled StudyCrystalline MaterialsEnergy-TransportEnergy ConversionEnergy MigrationEnergy TransferEthynylExciton MigrationExcitonsFluorescenceFluorescence QuenchingHarvestingHigh AnisotropyJava Programming LanguageLightLight-HarvestingLight-Harvesting SystemMetal Organic FrameworkMetalloporphyrinsMolecular StructureOrganometallic CompoundsPentafluorophenylPhotogenerated ExcitonsPhotosynthesisPorphyrinPorphyrin MoleculesPorphyrinsPyridylRelated CompoundsSolar EnergyStrutsTheoretical CalculationsTheoretical ModelUltra-FastUltra-Fast Energy MigrationUnclassified DrugZincZinc Compounds
Given that energy (exciton) migration in natural photosynthesis primarily occurs in highly ordered porphyrin-like pigments (chlorophylls), equally highly ordered porphyrin-based metal-organic frameworks (MOFs) might be expected to exhibit similar behavior, thereby facilitating antenna-like light-harvesting and positioning such materials for use in solar energy conversion schemes. Herein, we report the first example of directional, long-distance energy migration within a MOF. Two MOFs, namely F-MOF and DA-MOF that are composed of two Zn(II) porphyrin struts [5,15-dipyridyl-10,20-bis(pentafluorophenyl)porphinato]zinc(II) and [5,15-bis[4-(pyridyl)ethynyl]-10,20-diphenylporphinato]zinc(II), respectively, were investigated. From fluorescence quenching experiments and theoretical calculations, we find that the photogenerated exciton migrates over a net distance of up to ∼45 porphyrin struts within its lifetime in DA-MOF (but only ∼3 in F-MOF), with a high anisotropy along a specific direction. The remarkably efficient exciton migration in DA-MOF is attributed to enhanced π-conjugation through the addition of two acetylene moieties in the porphyrin molecule, which leads to greater Q-band absorption intensity and much faster exciton-hopping (energy transfer between adjacent porphyrin struts). The long distance and directional energy migration in DA-MOF suggests promising applications of this compound or related compounds in solar energy conversion schemes as an efficient light-harvesting and energy-transport component. © 2012 American Chemical Society.
American Chemical Society
Related Researcher
  • Author Jeong, Nak Cheon NC(Nanoporous-materials Chemistry for Fundamental Science) Lab
  • Research Interests Inorganic Chemistry; Metal-Organic Framework; Nanoporous Materials; Electron Transport;Ion Transport
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Department of Emerging Materials ScienceNC(Nanoporous-materials Chemistry for Fundamental Science) Lab1. Journal Articles

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