skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Exciton Migration and Amplified Quenching on Two-Dimensional Metal–Organic Layers

Abstract

The dimensionality dependency of resonance energy transfer is of great interest due to its importance in understanding energy transfer on cell membranes and in low-dimension nanostructures. Light harvesting two-dimensional metal–organic layers (2D-MOLs) and three-dimensional metal–organic frameworks (3D-MOFs) provide comparative models to study such dimensionality dependence with molecular accuracy. Here we report the construction of 2D-MOLs and 3D-MOFs from a donor ligand 4,4',4''-(benzene-1,3,5-triyl-tris(ethyne-2,1-diyl))tribenzoate (BTE) and a doped acceptor ligand 3,3',3''-nitro-4,4',4''-(benzene-1,3,5-triyl-tris(ethyne-2,1-diyl))tribenzoate (BTE-NO2). These 2D-MOLs and 3D-MOFs are connected by similar hafnium clusters, with key differences in the topology and dimensionality of the metal–ligand connection. Energy transfer from donors to acceptors through the 2D-MOL or 3D-MOF skeletons is revealed by measuring and modeling the fluorescence quenching of the donors. We found that energy transfer in 3D-MOFs is more efficient than that in 2D-MOLs, but excitons on 2D-MOLs are more accessible to external quenchers as compared with those in 3D-MOFs. These results not only provide support to theoretical analysis of energy transfer in low dimensions, but also present opportunities to use efficient exciton migration in 2D materials for light-harvesting and fluorescence sensing.

Authors:
; ; ; ; ; ; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
FOREIGN
OSTI Identifier:
1379432
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of the American Chemical Society; Journal Volume: 139; Journal Issue: 20
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Cao, Lingyun, Lin, Zekai, Shi, Wenjie, Wang, Zi, Zhang, Cankun, Hu, Xuefu, Wang, Cheng, and Lin, Wenbin. Exciton Migration and Amplified Quenching on Two-Dimensional Metal–Organic Layers. United States: N. p., 2017. Web. doi:10.1021/jacs.7b02470.
Cao, Lingyun, Lin, Zekai, Shi, Wenjie, Wang, Zi, Zhang, Cankun, Hu, Xuefu, Wang, Cheng, & Lin, Wenbin. Exciton Migration and Amplified Quenching on Two-Dimensional Metal–Organic Layers. United States. doi:10.1021/jacs.7b02470.
Cao, Lingyun, Lin, Zekai, Shi, Wenjie, Wang, Zi, Zhang, Cankun, Hu, Xuefu, Wang, Cheng, and Lin, Wenbin. Wed . "Exciton Migration and Amplified Quenching on Two-Dimensional Metal–Organic Layers". United States. doi:10.1021/jacs.7b02470.
@article{osti_1379432,
title = {Exciton Migration and Amplified Quenching on Two-Dimensional Metal–Organic Layers},
author = {Cao, Lingyun and Lin, Zekai and Shi, Wenjie and Wang, Zi and Zhang, Cankun and Hu, Xuefu and Wang, Cheng and Lin, Wenbin},
abstractNote = {The dimensionality dependency of resonance energy transfer is of great interest due to its importance in understanding energy transfer on cell membranes and in low-dimension nanostructures. Light harvesting two-dimensional metal–organic layers (2D-MOLs) and three-dimensional metal–organic frameworks (3D-MOFs) provide comparative models to study such dimensionality dependence with molecular accuracy. Here we report the construction of 2D-MOLs and 3D-MOFs from a donor ligand 4,4',4''-(benzene-1,3,5-triyl-tris(ethyne-2,1-diyl))tribenzoate (BTE) and a doped acceptor ligand 3,3',3''-nitro-4,4',4''-(benzene-1,3,5-triyl-tris(ethyne-2,1-diyl))tribenzoate (BTE-NO2). These 2D-MOLs and 3D-MOFs are connected by similar hafnium clusters, with key differences in the topology and dimensionality of the metal–ligand connection. Energy transfer from donors to acceptors through the 2D-MOL or 3D-MOF skeletons is revealed by measuring and modeling the fluorescence quenching of the donors. We found that energy transfer in 3D-MOFs is more efficient than that in 2D-MOLs, but excitons on 2D-MOLs are more accessible to external quenchers as compared with those in 3D-MOFs. These results not only provide support to theoretical analysis of energy transfer in low dimensions, but also present opportunities to use efficient exciton migration in 2D materials for light-harvesting and fluorescence sensing.},
doi = {10.1021/jacs.7b02470},
journal = {Journal of the American Chemical Society},
number = 20,
volume = 139,
place = {United States},
year = {Wed May 10 00:00:00 EDT 2017},
month = {Wed May 10 00:00:00 EDT 2017}
}