Organic-inorganic metal-halide layered perovskites are promising candidates for optoelectronics due to their tunable photoluminescence, strong excitonic binding energy (>200meV), and improved environmental stability compared to 3D perovskites. These materials can exhibit properties such as ferroelectricity, chirality, and room-temperature white light emission, among others. However, most advancements have been limited to lead-based structures, making the exploration of lead-free alternatives and the tuning of their optical properties a continuing challenge. This thesis first explores a solvent engineering approach to achieve white light emission in lead-based hybrid layered perovskites. By varying the solvent used during synthesis, we examine how the choice of the solvent affects the structure and morphology of this class of perovskite structure when using organic cations with different molecular configurations, including those with aromatic group. The intricate interaction between polar solvents and rigid aromatic organic cation shifts the photoluminescence (PL) spectrum from narrow blue emission with low PL quantum yield (PLQY) to broadband emission with a PLQY of up to 21% and a color rendering index above 80, indicating a potential for indoor and outdoor illumination. Next, we develop a straightforward method to synthesize tin-based organic-inorganic layered structures, aiming to streamline the screening and optimization process for a broader range of organic cations. By introducing organic cations with heteroatoms, we prepare structures with varied Sn-Br octahedral connectivity, ranging from disconnected to face-sharing octahedra, preserving the intercalation of organic layers. These structural variations result in tunable color coordinates from yellow-orange to bluish-green and PLQY up to 80%. This works denote the relevance of organic cations on the resulting structures and thus, the tunability of their optical properties. Finally, considering the vast parameter space involved in the synthesis of organic-inorganic metal-halide layered perovskites, we explore the emerging field of accelerated material discovery by using automated synthesis and data processing tools. We aim to investigate the ideal synthetic conditions to obtain efficient white light emission in organic-inorganic metal-halide layered perovskites.

Developing Hybrid Metal-Halide Layered perovskites and Derivatives for Optoelectronics

XXX, AARYAPRABHAKARAN
2024-10-02

Abstract

Organic-inorganic metal-halide layered perovskites are promising candidates for optoelectronics due to their tunable photoluminescence, strong excitonic binding energy (>200meV), and improved environmental stability compared to 3D perovskites. These materials can exhibit properties such as ferroelectricity, chirality, and room-temperature white light emission, among others. However, most advancements have been limited to lead-based structures, making the exploration of lead-free alternatives and the tuning of their optical properties a continuing challenge. This thesis first explores a solvent engineering approach to achieve white light emission in lead-based hybrid layered perovskites. By varying the solvent used during synthesis, we examine how the choice of the solvent affects the structure and morphology of this class of perovskite structure when using organic cations with different molecular configurations, including those with aromatic group. The intricate interaction between polar solvents and rigid aromatic organic cation shifts the photoluminescence (PL) spectrum from narrow blue emission with low PL quantum yield (PLQY) to broadband emission with a PLQY of up to 21% and a color rendering index above 80, indicating a potential for indoor and outdoor illumination. Next, we develop a straightforward method to synthesize tin-based organic-inorganic layered structures, aiming to streamline the screening and optimization process for a broader range of organic cations. By introducing organic cations with heteroatoms, we prepare structures with varied Sn-Br octahedral connectivity, ranging from disconnected to face-sharing octahedra, preserving the intercalation of organic layers. These structural variations result in tunable color coordinates from yellow-orange to bluish-green and PLQY up to 80%. This works denote the relevance of organic cations on the resulting structures and thus, the tunability of their optical properties. Finally, considering the vast parameter space involved in the synthesis of organic-inorganic metal-halide layered perovskites, we explore the emerging field of accelerated material discovery by using automated synthesis and data processing tools. We aim to investigate the ideal synthetic conditions to obtain efficient white light emission in organic-inorganic metal-halide layered perovskites.
2-ott-2024
File in questo prodotto:
File Dimensione Formato  
phdunige_4949507.pdf

accesso aperto

Tipologia: Tesi di dottorato
Dimensione 7.82 MB
Formato Adobe PDF
7.82 MB Adobe PDF Visualizza/Apri

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11567/1206815
Citazioni
  • ???jsp.display-item.citation.pmc??? ND
  • Scopus ND
  • ???jsp.display-item.citation.isi??? ND
social impact