Synthesis of BaZrS3 and BaHfS3 Chalcogenide Perovskite Films Using Single‐Phase Molecular Precursors at Moderate Temperatures. Issue 15 (6th March 2023)

• Record Type: Journal Article
• Authors: Pradhan, Apurva A.; Uible, Madeleine C.; Agarwal, Shubhanshu; Turnley, Jonathan W.; Khandelwal, Shriya; Peterson, Jonas M.; Blach, Daria D.; Swope, Ryan N.; Huang, Libai; Bart, Suzanne C.; Agrawal, Rakesh
• Is Part Of: Angewandte Chemie international edition. Volume 62:Issue 15(2023)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2023-03-06
• Subjects: Chalcogenide -- Dithiocarbamates -- Perovskites -- Solution Processing -- Transition Metals; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202301049
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: Chalcogenide perovskites have garnered interest for applications in semiconductor devices due to their excellent predicted optoelectronic properties and stability. However, high synthesis temperatures have historically made these materials incompatible with the creation of photovoltaic devices. Here, we demonstrate the solution processed synthesis of luminescent BaZrS3 and BaHfS3 chalcogenide perovskite films using single‐phase molecular precursors at sulfurization temperatures of 575 °C and sulfurization times as short as one hour. These molecular precursor inks were synthesized using known carbon disulfide insertion chemistry to create Group 4 metal dithiocarbamates, and this chemistry was extended to create species, such as barium dithiocarboxylates, that have never been reported before. These findings, with added future research, have the potential to yield fully solution processed thin films of chalcogenide perovskites for various optoelectronic applications. Abstract : We have developed a single‐phase, solution‐processed approach to create thin films of BaZrS3 and BaHfS3 at temperatures of 575 °C with sulfurization times as short as 20 min. To create molecular precursor inks, we utilized known carbon disulfide insertion chemistry to synthesize Group 4 metal dithiocarbamates and extended this chemistry to create species such as barium dithiocarboxylates, that have not been reported before.