Organosilicon-Based Ligand Design for High-Performance Perovskite Nanocrystal Films for Color Conversion and X‑ray Imaging

• Published in: ACS nano Vol. 18; no. 14; pp. 10054 - 10062
• Main Authors: Chen, Junchi, Jiang, Guocan, Hamann, Elias, Mescher, Henning, Jin, Qihao, Allegro, Isabel, Brenner, Philipp, Li, Zhengquan, Gaponik, Nikolai, Eychmüller, Alexander, Lemmer, Uli
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 09.04.2024
• Subjects: film formation; scintillator; ligand design; organosilicon ligands; reduced scattering; perovskite nanocrystals; X-ray imaging
• ISSN: 1936-0851; 1936-086X
• DOI: 10.1021/acsnano.3c11991

Perovskite nanocrystals (PNCs) bear a huge potential for widespread applications, such as color conversion, X-ray scintillators, and active laser media. However, the poor intrinsic stability and high susceptibility to environmental stimuli including moisture and oxygen have become bottlenecks of PNC materials for commercialization. Appropriate barrier material design can efficiently improve the stability of the PNCs. Particularly, the strategy for packaging PNCs in organosilicon matrixes can integrate the advantages of inorganic-oxide-based and polymer-based encapsulation routes. However, the inert long-carbon-chain ligands (e.g., oleic acid, oleylamine) used in the current ligand systems for silicon-based encapsulation are detrimental to the cross-linking of the organosilicon matrix, resulting in performance deficiencies in the nanocrystal films, such as low transparency and large surface roughness. Herein, we propose a dual-organosilicon ligand system consisting of (3-aminopropyl)­triethoxysilane (APTES) and (3-aminopropyl)­triethoxysilane with pentanedioic anhydride (APTES-PA), to replace the inert long-carbon-chain ligands for improving the performance of organosilicon-coated PNC films. As a result, strongly fluorescent PNC films prepared by a facile solution-casting method demonstrate high transparency and reduced surface roughness while maintaining high stability in various harsh environments. The optimized PNC films were eventually applied in an X-ray imaging system as scintillators, showing a high spatial resolution above 20 lp/mm. By designing this promising dual organosilicon ligand system for PNC films, our work highlights the crucial influence of the molecular structure of the capping ligands on the optical performance of the PNC film.