Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 56, Issue 46, Pages 14743-14748Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201706492
Keywords
charge polarization; metal-organic frameworks; nonlinear optics; photon upconversion; TD-DFT calculations
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Funding
- Alexander von Humboldt foundation
- German Federal Ministry of Education and Research (BMBF) [01IH15001]
- Singapore Ministry of Education [MOE2011-T3-1-005]
- NCN [UMO-2013/10/A/ST4/00114]
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Multi-photon absorption (MPA) is among the most prominent nonlinear optical (NLO) effects and has applications, for example in telecommunications, defense, photonics, and bio-medicines. Established MPA materials include dyes, quantum dots, organometallics and conjugated polymers, most often dispersed in solution. We demonstrate how metalorganic frameworks (MOFs), a novel NLO solid-state materials class, can be designed for exceptionally strong MPA behavior. MOFs consisting of zirconium-and hafnium-oxoclusters and featuring a chromophore linker based on the tetraphenylethene (TPE) molecule exhibit record high two-photon absorption (2PA) cross-section values, up to 3600 GM. The unique modular building-block principle of MOFs allows enhancing and optimizing their MPA properties in a theory-guided approach by combining tailored charge polarization, conformational strain, three-dimensional arrangement, and alignment of the chromophore linkers in the crystal.
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