• Sponseller, Melany
• Bulovic, Vladimir
• Farnaz, Niroui
• Jung, Young-Kwang
• Stan, Camelia
• Li, Yao
• Stranks, Samuel
• Alsari, Mejd
• Brenes, Roberto
• Abdi-Jalebi, Mojtaba
• Macdonald, J. Emyr
• Duck, Benjamin
• Friend, Richard
• Lilliu, Samuele
• Walsh, Aron
• Settens, Charles
• Burghammer, Manfred
• Osherov, Anna
• Tamura, Nobumichi

Abstract

Halide perovskites are promising semiconductors for inexpensive, high-performance optoelectronics. Despite a remarkable defect tolerance compared to conventional semiconductors, perovskite thin films still show substantial microscale heterogeneity in key properties such as luminescence efficiency and device performance1, 2, 3. This behavior has been attributed to spatial fluctuations in the population of sub-bandgap electronic states that act as trap-mediated non-radiative recombination sites.1, 4 However, the origin of the variations, trap states and extent of the defect tolerance remains a topic of debate, and a precise understanding is critical to the rational design of defect management strategies.5, 6 By combining scanning X-ray diffraction beamlines at two different synchrotrons with high-resolution transmission electron microscopy, we reveal levels of heterogeneity on the ten-micrometer scale (super-grains) and even ten-nanometer scale (sub-grain domains). We find that local strain is associated with enhanced defect concentrations, and correlations between the local structure and time-resolved photoluminescence reveal that these strain-related defects are the cause of non-radiative recombination. We reveal a direct connection between defect concentrations and non-radiative losses, as well as complex heterogeneity across multiple length scales, shedding new light on the presence and influence of structural defects in halide perovskites.

Topics

• perovskite
• impedance spectroscopy
• photoluminescence
• grain
• x-ray diffraction
• thin film
• semiconductor
• transmission electron microscopy
• defect