Experimental and Theoretical Investigation on the Temperature-dependent Optical Properties of Hybrid Halide Perovskites

dc.contributor.advisorSchwingenschlögl, Udo
dc.contributor.authorAlharbi, Ohoud K.
dc.contributor.committeememberLaquai, Frédéric
dc.contributor.committeememberLanza, Mario
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.date.accessioned2022-09-04T08:49:11Z
dc.date.available2022-09-04T08:49:11Z
dc.date.issued2022-08-30
dc.description.abstractNowadays, 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.
dc.identifier.citationAlharbi, O. K. (2022). Experimental and Theoretical Investigation on the Temperature-dependent Optical Properties of Hybrid Halide Perovskites [KAUST Research Repository]. https://doi.org/10.25781/KAUST-94BU7
dc.identifier.doi10.25781/KAUST-94BU7
dc.identifier.orcid0000-0002-3903-2144
dc.identifier.urihttp://hdl.handle.net/10754/680834
dc.language.isoen
dc.person.id173448
dc.subjectPerovskites
dc.subjectDensity Functional Theory
dc.subjectOptical properties
dc.titleExperimental and Theoretical Investigation on the Temperature-dependent Optical Properties of Hybrid Halide Perovskites
dc.typeThesis
display.details.left<span><h5>Type</h5>Thesis<br><br><h5>Authors</h5><a href="https://repository.kaust.edu.sa/search?query=orcid.id:0000-0002-3903-2144&spc.sf=dc.date.issued&spc.sd=DESC">Alharbi, Ohoud K.</a> <a href="https://orcid.org/0000-0002-3903-2144" target="_blank"><img src="https://repository.kaust.edu.sa/server/api/core/bitstreams/82a625b4-ed4b-40c8-865a-d6a5225a26a4/content" width="16" height="16"/></a><br><br><h5>Advisors</h5><a href="https://repository.kaust.edu.sa/search?query=orcid.id:0000-0003-4179-7231&spc.sf=dc.date.issued&spc.sd=DESC">Schwingenschlögl, Udo</a> <a href="https://orcid.org/0000-0003-4179-7231" target="_blank"><img src="https://repository.kaust.edu.sa/server/api/core/bitstreams/82a625b4-ed4b-40c8-865a-d6a5225a26a4/content" width="16" height="16"/></a><br><br><h5>Committee Members</h5><a href="https://repository.kaust.edu.sa/search?query=orcid.id:0000-0002-5887-6158&spc.sf=dc.date.issued&spc.sd=DESC">Laquai, Frédéric</a> <a href="https://orcid.org/0000-0002-5887-6158" target="_blank"><img src="https://repository.kaust.edu.sa/server/api/core/bitstreams/82a625b4-ed4b-40c8-865a-d6a5225a26a4/content" width="16" height="16"/></a><br><a href="https://repository.kaust.edu.sa/search?query=orcid.id:0000-0003-4756-8632&spc.sf=dc.date.issued&spc.sd=DESC">Lanza, Mario</a> <a href="https://orcid.org/0000-0003-4756-8632" target="_blank"><img src="https://repository.kaust.edu.sa/server/api/core/bitstreams/82a625b4-ed4b-40c8-865a-d6a5225a26a4/content" width="16" height="16"/></a><br><br><h5>Program</h5><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.program=Applied Physics,equals">Applied Physics</a><br><br><h5>KAUST Department</h5><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.department=Physical Science and Engineering (PSE) Division,equals">Physical Science and Engineering (PSE) Division</a><br><br><h5>Date</h5>2022-08-30</span>
display.details.right<span><h5>Abstract</h5>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.<br><br><h5>Citation</h5>Alharbi, O. K. (2022). Experimental and Theoretical Investigation on the Temperature-dependent Optical Properties of Hybrid Halide Perovskites [KAUST Research Repository]. https://doi.org/10.25781/KAUST-94BU7<br><br><h5>DOI</h5><a href="https://doi.org/10.25781/KAUST-94BU7">10.25781/KAUST-94BU7</a></span>
kaust.availability.selectionRelease the work immediately for public access* on the internet through the KAUST Repository.
kaust.gpcmazen.mero@kaust.edu.sa
kaust.request.doiyes
kaust.thesis.advisorApprovalRequestedYes, I have already submitted the final approval form to my advisor.
orcid.id0000-0003-4756-8632
orcid.id0000-0002-5887-6158
orcid.id0000-0003-4179-7231
orcid.id0000-0002-3903-2144
refterms.dateFOA2022-09-04T08:49:11Z
thesis.degree.disciplineApplied Physics
thesis.degree.grantorKing Abdullah University of Science and Technology
thesis.degree.nameMaster of Science
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