Quantum mechanics

Chemical physics

Materials science

Perovskite (structure)

Semiconductor

Grain boundary

Thermodynamics

Grain size

Physics

Nanotechnology

Diffusion

Microstructure

Charge carrier

Cathodoluminescence

Luminescence

Thin film

Condensed matter physics

Composite material

Charge (physics)

Crystallography

Chemistry

Optoelectronics

Advanced Functional Materials

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, Cs 2 AgBiBr 6 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 Cs 2 AgBiBr 6 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 &gt;1 µm found in Cs 2 AgBiBr 6 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.

Understanding the Role of Grain Boundaries on Charge‐Carrier and Ion Transport in Cs<sub>2</sub>AgBiBr<sub>6</sub> Thin Films

Understanding the Role of Grain Boundaries on Charge‐Carrier and Ion Transport in Cs2AgBiBr6 Thin Films

Understanding the Role of Grain Boundaries on Charge‐Carrier and Ion Transport in Cs₂AgBiBr₆ Thin Films