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

Title
Light-Harvesting and Ultrafast Energy Migration in Porphyrin-Based Metal-Organic Frameworks
Authors
Son, HJ[Son, Ho-Jin]Jin, SY[Jin, Shengye]Patwardhan, S[Patwardhan, Sameer]Wezenberg, SJ[Wezenberg, Sander J.]Jeong, NC[Jeong, Nak Cheon]So, M[So, Monica]Wilmer, CE[Wilmer, Christopher E.]Sarjeant, AA[Sarjeant, Amy A.]Schatz, GC[Schatz, George C.]Snurr, RQ[Snurr, Randall Q.]Farha, OK[Farha, Omar K.]Wiederrecht, GP[Wiederrecht, Gary P.]Hupp, JT[Hupp, Joseph T.]
DGIST Authors
Jeong, NC[Jeong, Nak Cheon]
Issue Date
2013-01-16
Citation
Journal of the American Chemical Society, 135(2), 862-869
Type
Article
Article Type
Article
Keywords
[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
ISSN
0002-7863
Abstract
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.
URI
http://hdl.handle.net/20.500.11750/3267
DOI
10.1021/ja310596a
Publisher
American Chemical Society
Files:
There are no files associated with this item.
Collection:
Emerging Materials ScienceETC1. Journal Articles


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