In this paper, we present spectroscopic ellipsometry measurements of (MA0.13FA0.87)PbI3 single crystals assessed at photon energies of 0.73–6.42 eV and at temperatures between 4.4 and 400 K. At room temperature, the refractive index was dispersed as a function of frequency, which is typical of a semiconductor. The absorption spectrum exhibited several electronic transitions. We estimated a room temperature direct band gap of 1.66 ± 0.02 eV and exciton binding energy of 40 meV. With decreasing temperature, the refractive index increased. The room-temperature thermo-optic coefficients were −1.7 × 10−4 and −2.5 × 10−4 K−1 at wavelength of 600 and 1200 nm. The exciton peak position and bandgap energy exhibited a redshift, which was attributed to a reverse ordering of the band structures. Additionally, an anomaly in exciton peak position and bandgap occurred at approximately 100–200 K due to the structural phase transition. This phenomenon was associated with the coexistence of MA/FA-disordered and MA/FA-ordered domains. Our results provide a foundation for the technological development of lead halide perovskites-based photonic devices at various temperatures.
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