Directional Exciton Migration in Benzoimidazole-Based Metal–Organic Frameworks
AuthorsGutierrez Arzaluz, Luis
Mohammed, Omar F.
KAUST DepartmentPhysical Science and Engineering (PSE) Division
Advanced Membranes and Porous Materials Research Center
Material Science and Engineering Program
KAUST Catalysis Center (KCC)
Chemical Science Program
KAUST Solar Center (KSC)
KAUST Grant NumberCARF-FCC/1/1972-63-01
Embargo End Date2022-05-19
Permanent link to this recordhttp://hdl.handle.net/10754/669251
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AbstractHighly luminescent metal-organic frameworks (MOFs) have recently received great attention due to their potential applications as sensors and light-emitting devices. In these MOFs, the highly ordered fluorescent organic linkers positioning prevents excited-state self-quenching and rotational motion, enhancing their light-harvesting properties. Here, the exciton migration between the organic linkers with the same chemical structure but different protonation degrees in Zr-based MOFs was explored and deciphered using ultrafast laser spectroscopy and density functional theory calculations. First, we clearly demonstrate how hydrogen-bonding interactions between free linkers and solvents affect the twisting changes, internal conversion processes, and luminescent behavior of a benzoimidazole-based linker. Second, we provide clear evidence of an ultrafast energy transfer between well-aligned adjacent linkers with different protonation states inside the MOF. These findings provide a new fundamental photophysical insight into the exciton migration dynamics between linkers with different protonation states coexisting at different locations in MOFs and serve as a benchmark for improving light-harvesting MOF architectures.
CitationGutiérrez-Arzaluz, L., Jia, J., Gu, C., Czaban-Jóźwiak, J., Yin, J., Shekhah, O., … Mohammed, O. F. (2021). Directional Exciton Migration in Benzoimidazole-Based Metal–Organic Frameworks. The Journal of Physical Chemistry Letters, 4917–4927. doi:10.1021/acs.jpclett.1c01053
SponsorsThe authors thank King Abdullah University of Science and Technology (KAUST) and the CARF-FCC/1/1972-63-01 project for financial support and the Supercomputing Laboratory at KAUST for computational and storage resources.
PublisherAmerican Chemical Society (ACS)
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