Giant Enhancement of Second Harmonic Generation Accompanied by the Structural Transformation of 7‐Fold to 8‐Fold Interpenetrated Metal–Organic Frameworks (MOFs)

Interpenetration in metal–organic frameworks (MOFs) is an intriguing phenomenon with significant impacts on their properties, and functional applications. Herein, we show that a 7‐fold interpenetrated MOF (1) is transformed into an 8‐fold interpenetrated MOF by the loss of DMF in a single‐crystal‐to...

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Published in:Angewandte Chemie 2020-01, Vol.132 (2), p.843-848
Main Authors: Chen, Zhihui, Gallo, Gianpiero, Sawant, Vaishali A., Zhang, Tianxiang, Zhu, Menglong, Liang, Liangliang, Chanthapally, Anjana, Bolla, Geetha, Quah, Hong Sheng, Liu, Xiaogang, Loh, Kian Ping, Dinnebier, Robert E., Xu, Qing‐Hua, Vittal, Jagadese J.
Format: Article
Language:English
Subjects:
Chemistry
Crystals
Diamonds
Dipole moments
Einkristall-Einkristall-Umwandlung
Frequenzverdopplung
Metal-organic frameworks
Metall-organische Gerüste
Nichtlineare Optik
Photoluminescence
Photons
Second harmonic generation
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Summary:Interpenetration in metal–organic frameworks (MOFs) is an intriguing phenomenon with significant impacts on their properties, and functional applications. Herein, we show that a 7‐fold interpenetrated MOF (1) is transformed into an 8‐fold interpenetrated MOF by the loss of DMF in a single‐crystal‐to‐single‐crystal manner. This is accompanied by a giant enhancement of the second harmonic generation (SHG ca. 125 times) and two‐photon photoluminescence (ca. 14 times). The strengthened π–π interaction between the individual diamondoid networks and intensified oscillator strength of the molecules aid the augment of dipole moments and boost the nonlinear optical conversion efficiency. Large positive and negative thermal expansions of 1 occur at 30–150 °C before the loss of DMF. These results offer an avenue to manipulate the NLO properties of MOFs using interpenetration and provide access to tunable single‐crystal NLO devices. NLO‐MOFs: Eine Transformation von einem 7‐fach zu einem 8‐fach verzahnten Metall‐organischen Gerüst unter Verlust von DMF geht mit einem starken Anstieg der Frequenzverdopplung (SHG) und der Zwei‐Photonen‐Emission durch die erhöhte π‐π‐Interaktion und Oszillatorstärke einher. Somit können die nichtlinearen optischen (NLO) Eigenschaften von MOFs durch Interpenetration manipuliert werden.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.201911632