Static Disorder in Lead Halide Perovskites

J Phys Chem Lett. 2022 Aug 11;13(31):7280-7285. doi: 10.1021/acs.jpclett.2c01652. Epub 2022 Aug 2.

Abstract

In crystalline and amorphous semiconductors, the temperature-dependent Urbach energy can be determined from the inverse slope of the logarithm of the absorption spectrum and reflects the static and dynamic energetic disorder. Using recent advances in the sensitivity of photocurrent spectroscopy methods, we elucidate the temperature-dependent Urbach energy in lead halide perovskites containing different numbers of cation components. We find Urbach energies at room temperature to be 13.0 ± 1.0, 13.2 ± 1.0, and 13.5 ± 1.0 meV for single, double, and triple cation perovskite. Static, temperature-independent contributions to the Urbach energy are found to be as low as 5.1 ± 0.5, 4.7 ± 0.3, and 3.3 ± 0.9 meV for the same systems. Our results suggest that, at a low temperature, the dominant static disorder in perovskites is derived from zero-point phonon energy rather than structural disorder. This is unusual for solution-processed semiconductors but broadens the potential application of perovskites further to quantum electronics and devices.