Understanding the Role of Grain Boundaries on Charge‐Carrier and Ion Transport in Cs2AgBiBr6 Thin Films. (4th September 2021)

• Record Type: Journal Article
• Authors: Li, Zewei; Senanayak, Satyaprasad P.; Dai, Linjie; Kusch, Gunnar; Shivanna, Ravichandran; Zhang, Youcheng; Pradhan, Dipika; Ye, Junzhi; Huang, Yi‐Teng; Sirringhaus, Henning; Oliver, Rachel A.; Greenham, Neil C.; Friend, Richard H.; Hoye, Robert L. Z.
• Is Part Of: Advanced functional materials. Volume 31:Number 49(2021)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2021-09-04
• Subjects: carrier mobilities -- grain boundaries -- ion migration -- lead‐free double perovskites -- thin film transistors; Materials -- Periodicals; Chemical vapor deposition -- Periodicals; 620.11
• DOI: 10.1002/adfm.202104981
• Languages: English
• ISSNs: 1616-301X

Abstract

Abstract: Halide double perovskites have gained significant attention, owing to their composition of low‐toxicity elements, stability in air, and recent demonstrations of long charge‐carrier lifetimes that can exceed 1 µs. In particular, Cs2 AgBiBr6 is the subject of many investigations in photovoltaic devices. However, the efficiencies of solar cells based on this double perovskite are still far from the theoretical efficiency limit of the material. Here, the role of grain size on the optoelectronic properties of Cs2 AgBiBr6 thin films is investigated. It is shown through cathodoluminescence measurements that grain boundaries are the dominant nonradiative recombination sites. It also demonstrates through field‐effect transistor and temperature‐dependent transient current measurements that grain boundaries act as the main channels for ion transport. Interestingly, a positive correlation between carrier mobility and temperature is found, which resembles the hopping mechanism often seen in organic semiconductors. These findings explain the discrepancy between the long diffusion lengths >1 µm found in Cs2 AgBiBr6 single crystals versus the limited performance achieved in their thin film counterparts. This work shows that mitigating the impact of grain boundaries will be critical for these double perovskite thin films to reach the performance achievable based on their intrinsic single‐crystal properties. Abstract : Cs2 AgBiBr6 has gained attention as a lead‐free, stable perovskite. However, the transport properties in thin films have significantly fallen short of their single crystal counterparts. Herein, through cathodoluminescence mapping measurements and by developing the first double perovskite field‐effect transistors, grain boundaries are identified to be a key limiting factor, acting as the dominant sites for nonradiative recombination and ion migration.