Refractive index change dominates the transient absorption response of metal halide perovskite thin films in the near infrared

Abstract

Perovskites have lately attracted a lot of attention as promising materials for the next-generation of efficient, low-cost, and solution processable optoelectronics. Their complex transient photophysics, in time scales ranging from femtoseconds to seconds, have been widely investigated. However, in most of the reported works the spectral window of ultrafast transient absorption (TA) spectroscopy of perovskite films is limited to the visible region, hence missing crucial information coming from the near-infrared (NIR). Furthermore, the measured TA responses are affected by light interference in a thin perovskite layer making data interpretation a challenge even in the visible part of the spectrum. Here, we demonstrate a method that allows us to separately obtain the changes in absorption and refractive index from conventional transmission and reflection pump-probe measurements. We show that the contribution of the absorption change to the response of metal halide perovskite thin films in the NIR is much smaller than that of the refractive index change. Furthermore, the spectral shape of TA responses in the NIR range is predominantly determined by perovskite layer thickness and its refractive index. However, the time profile of the responses bears important information on the carrier dynamics and makes the NIR a useful range to study perovskite photophysics.