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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, 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
- 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); Absorption; Absorption Intensity; Acetylene; Acetylene Derivative; Addition Reaction; Anisotropy; Antenna; Calculation; Chlorophyll; Conjugation; Controlled Study; Crystalline Materials; Energy-Transport; Energy Conversion; Energy Migration; Energy Transfer; Ethynyl; Exciton Migration; Excitons; Fluorescence; Fluorescence Quenching; Harvesting; High Anisotropy; Java Programming Language; Light; Light-Harvesting; Light-Harvesting System; Metal Organic Framework; Metalloporphyrins; Molecular Structure; Organometallic Compounds; Pentafluorophenyl; Photogenerated Excitons; Photosynthesis; Porphyrin; Porphyrin Molecules; Porphyrins; Pyridyl; Related Compounds; Solar Energy; Struts; Theoretical Calculations; Theoretical Model; Ultra-Fast; Ultra-Fast Energy Migration; Unclassified Drug; Zinc; Zinc 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
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- Emerging Materials ScienceETC1. Journal Articles
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