Quantification of the ionic migration rates in thick CsPbBr3 films revealed by operando x-ray fluorescence

Abstract

Bulk CsPbBr3 is an emerging semiconductor that has shown unprecedented increase in performance over the last decade for optoelectronic applications. However, further development of devices based on CsPbBr3 is hampered by their poor electrical stability under operation. Migration and accumulation of native ions (Cs+, Pb2+, and Br-) under electric fields has been suggested by many groups to be responsible for the observed device instabilities, although direct experimental evidence of ionic motion during operation has been seldom reported. In our study, ion migration has been probed by grazing incidence x-ray fluorescence (GIXRF) in CsPbBr3 polycrystalline layers grown in vapor phase. Our findings indicate that both Cs and Br experience ionic migration under electric field, suggesting that these ions are responsible for the measured current instability in our devices. In the timescale of a few hours, the ionic drifting rates of mobile Cs and Br under the top electrode were found to be similar, as high as ∼ 20 ppm h−1 V−1 mm. This work paves the way for a better understanding of ion motion issues that play a key role in the optoelectronic properties of CsPbBr3 devices.