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Covalent Organic Framework Thin-Film Photodetectors from Solution-Processable Porous Nanospheres

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Title
Covalent Organic Framework Thin-Film Photodetectors from Solution-Processable Porous Nanospheres
Author(s)
Saikat Bag; Himadri Sekhar Sasmal; Sonu Pratap Chaudhary; Kaushik Dey; Dominic Blätte; Roman Guntermann; Yingying Zhang; Miroslav Položij; Agnieszka Kuc; Ankita Shelke; Ratheesh K. Vijayaraghavan; Thalasseril G. Ajithkumar; Sayan Bhattacharyya; Thomas Heine; Thomas Bein; Rahul Banerjee
Publication Date
2023-01
Journal
Journal of the American Chemical Society, v.145, no.3, pp.1649 - 1659
Publisher
American Chemical Society
Abstract
The synthesis of homogeneous covalent organic framework (COF) thin films on a desired substrate with decent crystallinity, porosity, and uniform thickness has great potential for optoelectronic applications. We have used a solution-processable sphere transmutation process to synthesize 300 ± 20 nm uniform COF thin films on a 2 × 2 cm2 TiO2-coated fluorine-doped tin oxide (FTO) surface. This process controls the nucleation of COF crystallites and molecular morphology that helps the nanospheres to arrange periodically to form homogeneous COF thin films. We have synthesized four COF thin films (TpDPP, TpEtBt, TpTab, and TpTta) with different functional backbones. In a close agreement between the experiment and density functional theory, the TpEtBr COF film showed the lowest optical band gap (2.26 eV) and highest excited-state lifetime (8.52 ns) among all four COF films. Hence, the TpEtBr COF film can participate in efficient charge generation and separation. We constructed optoelectronic devices having a glass/FTO/TiO2/COF-film/Au architecture, which serves as a model system to study the optoelectronic charge transport properties of COF thin films under dark and illuminated conditions. Visible light with a calibrated intensity of 100 mW cm−2 was used for the excitation of COF thin films. All of the COF thin films exhibit significant photocurrent after illumination with visible light in comparison to the dark. Hence, all of the COF films behave as good photoactive substrates with minimal pinhole defects. The fabricated out-of-plane photodetector device based on the TpEtBr COF thin film exhibits high photocurrent density (2.65 ± 0.24 mA cm−2 at 0.5 V) and hole mobility (8.15 ± 0.64 ×10−3 cm2 V−1 S−1 ) compared to other assynthesized films, indicating the best photoactive characteristics.
URI
https://pr.ibs.re.kr/handle/8788114/15889
DOI
10.1021/jacs.2c09838
ISSN
0002-7863
Appears in Collections:
Center for Nanomedicine (나노의학 연구단) > 1. Journal Papers (저널논문)
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