Nowadays, studying materials for renewable energy applications are highly de-
manded. Hybrid halide perovskites have proven to be promising materials for
such technology since their first application in solar cells in 2008, with a power
conversion efficiency of 2.7%. Since then, hybrid halide perovskites have proven
their superior properties for light-absorbing devices. In this scope, studying the
optical properties is ultimately essential. This work investigates the tempera-
ture dependence of the optical spectra for formamidinium lead iodide/bromide
perovskites (FAPb[IxBr1-x]3 (0 ≤ x ≤ 1) using spectroscopic ellipsometry mea-
surements, empirical optical modeling, density functional theory, and molecular
dynamics. Five FAPb[IxBr1-x]3 perovskite samples were fabricated by a hybrid
processing technique. External Quantum Efficiency measurements reported an
energy bandgap range between 1.58 eV and 1.77 eV for the resulted samples.
Next, multi-angle spectroscopic ellipsometry measurements were applied with a
temperature-controlled stage, allowing the variance of temperature from 25 ◦C to
75 ◦C. The results show a blue shift in the optical spectra at elevated tempera-
tures. We then conducted a temperature-dependent empirical model that predicts
the optical spectra for the sample of study at higher temperatures using input
data of the spectra at room temperature. The model reports low mean squared
errors which are less than ≈ 2 around the bandgap, and further development can
be applied for better utilization.
First-principles investigations were conducted on four FAPb[IxBr1-x]3 per-
ovskite unit cells. Structural optimization was applied with assuming fixed angles
of the lattice. Atomic configuration was chosen to achieve minimal ground state
energies. Ab initio molecular dynamics simulations were applied to each opti-
mized structures at target temperatures of 300 K and 350 K using Berendsen
thermostat. The simulation time was 4ps with 1fs time step, and the electronic
energy bandgap was calculated at each step using PBE functional. The simula-
tions reported a rotational motion for the FA molecule that showed to be faster
at 350 K, along with higher mean energy bandgap compared to the reported
value at 300 K. The optical spectra were extracted using a snapshot from the
resulted structures. Similar to the spectroscopic ellipsometry measurements, a
temperature induced blue shift was reported.
Overall, this work detects and predicts the temperature-dependent optical
spectra and confirms the role of the atomic thermal motion. With further devel-
opment, higher accuracy can be achieved along with broadening the materials of
study for photovoltaic and optoelectronic applications.
| Identifer | oai:union.ndltd.org:kaust.edu.sa/oai:repository.kaust.edu.sa:10754/680834 |
| Date | 30 August 2022 |
| Creators | Alharbi, Ohoud K. |
| Contributors | Schwingenschlögl, Udo, Physical Science and Engineering (PSE) Division, Laquai, Frédéric, Lanza, Mario |
| Source Sets | King Abdullah University of Science and Technology |
| Language | English |
| Detected Language | English |
| Type | Thesis |
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