Bederak Dmytro, Sukharevska Nataliia, Kahmann Simon, Abdu-Aguye Mustapha, Duim Herman, Dirin Dmitry N, Kovalenko Maksym V, Portale Giuseppe, Loi Maria A
Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 4, Groningen 9747AG, The Netherlands.
Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1, Zürich 8093, Switzerland.
ACS Appl Mater Interfaces. 2020 Nov 25;12(47):52959-52966. doi: 10.1021/acsami.0c16646. Epub 2020 Nov 11.
Phase-transfer exchange of pristine organic ligands for inorganic ones is essential for the integration of colloidal quantum dots (CQDs) in optoelectronic devices. This method results in a colloidal dispersion (ink) which can be directly deposited by various solution-processable techniques to fabricate conductive films. For PbS CQDs capped with methylammonium lead iodide ligands (MAPbI), the most commonly employed solvent is butylamine, which enables only a short-term (hours) colloidal stability and thus brings concerns on the possibility of manufacturing CQD devices on a large scale in a reproducible manner. In this work, we studied the stability of alternative inks in two highly polar solvents which impart long-term colloidal stability of CQDs: propylene carbonate (PC) and 2,6-difluoropyridine (DFP). The aging and the loss of the ink's stability were monitored with optical, structural, and transport measurements. With these solvents, PbS CQDs capped with MAPbI ligands retain colloidal stability for more than 20 months, both in dilute and concentrated dispersions. After 17 months of ink storage, transistors with a maximum linear mobility for electrons of 8.5 × 10 cm/V s are fabricated; this value is 17% of the one obtained with fresh solutions. Our results show that both PC- and DFP-based PbS CQD inks offer the needed shelf life to allow for the development of a CQD device technology.
将原始有机配体交换为无机配体的相转移过程对于胶体量子点(CQD)集成到光电器件中至关重要。这种方法会产生一种胶体分散液(油墨),可通过各种溶液可加工技术直接沉积以制造导电膜。对于用甲基碘化铅配体(MAPbI)封端的硫化铅CQD,最常用的溶剂是丁胺,它只能实现短期(数小时)的胶体稳定性,因此引发了对以可重复方式大规模制造CQD器件可能性的担忧。在这项工作中,我们研究了两种高极性溶剂中替代油墨的稳定性,这两种溶剂能赋予CQD长期胶体稳定性:碳酸丙烯酯(PC)和2,6 - 二氟吡啶(DFP)。通过光学、结构和传输测量来监测油墨的老化和稳定性损失。使用这些溶剂时,用MAPbI配体封端的硫化铅CQD在稀释和浓缩分散液中都能保持超过20个月的胶体稳定性。在油墨储存17个月后,制造出了电子最大线性迁移率为8.5×10 cm/V s的晶体管;该值是新鲜溶液所获值的17%。我们的结果表明,基于PC和DFP的硫化铅CQD油墨都提供了所需的保质期,以推动CQD器件技术的发展。