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Vibrational Paddlewheel Cu-Cu Node in Metal-Organic Frameworks: Probe of Nonradiative Relaxation

Title
Vibrational Paddlewheel Cu-Cu Node in Metal-Organic Frameworks: Probe of Nonradiative Relaxation
Authors
Song, Hye InBae, JinheeLee, Eun JiKirlikovali, K.O.Farha, O.K.Jeong, N.C.
DGIST Authors
Jeong, N.C.
Issue Date
2020-05
Citation
Journal of Physical Chemistry C, 124(24), 13187-13195
Type
Article
Article Type
Article
Keywords
Artificial moleculeContemporary chemistryMetalorganic frameworks (MOFs)Molecular interaction energyNon-radiative relaxationRaman measurementsSolvent moleculesThermal dissipationCopper compoundsBinary alloysDissociationKinetic energyKineticsMetal-Organic FrameworksMoleculesOrganometallicsSolventsThermal energy
ISSN
1932-7447
Abstract
Nonradiative relaxation, a ubiquitous phenomenon in natural and artificial molecules and materials, has been extensively studied in contemporary chemistry. In this report, we show the nonradiative relaxation of Cu(II)-based paddlewheel metal-organic frameworks (MOFs), HKUST-1 and Cu-MOF-2, with Raman measurements. Irradiation of the Cu-based MOF crystals by a 532 nm laser with the minimum power of 1.5-8.0 mW results in the dissociation of the axially ligated solvent molecules at the paddlewheel Cu(II) sites. Dissociation arises by the accumulated thermal energy formed by nonradiative relaxation, and the minimum power necessary is dependent on both the type of MOF and the Lewis basic solvent molecule that is coordinated to the metal node. We demonstrate that the minimum power is associated with an equilibrium between the accumulation and dissipation of thermal energy and also that thermal dissipation is dependent on the coordination strength, molecular interaction energy, and kinetic energy of the solvent molecules residing in the pores. Finally, we show the nonradiative relaxation behavior of nonluminescent MOFs based on the comparison between the Cu-based MOFs and Zn-MOF-2, a structurally analogous MOF that does not exhibit nonradiative relaxation. © 2020 American Chemical Society.
URI
http://hdl.handle.net/20.500.11750/12818
DOI
10.1021/acs.jpcc.0c02255
Publisher
American Chemical Society
Related Researcher
  • Author Jeong, Nak Cheon Supramolecular Inorganic Chemistry Laboratory
  • Research Interests Inorganic Chemistry; Metal-Organic Framework; Nanoporous Materials; Electron Transport;Ion Transport
Files:
There are no files associated with this item.
Collection:
Department of Emerging Materials ScienceSupramolecular Inorganic Chemistry Laboratory1. Journal Articles


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