Engineering of Lead-Free Materials for Light-Emitting Application: Structural and Photophysical Studies

  • Jawaher Almutlaq

Student thesis: Doctoral Thesis

Abstract

Finding luminescent materials with narrow-band emissions, high stability, and high photoluminescence quantum yield (PLQY), yet relatively fast radiative decay rates, has been an outstanding research challenge. This thesis aims to develop different luminescent materials and examine their structural and optical properties for light-emitting applications. The first part of this thesis covers the controversy regarding the origin of emission in zerodimensional perovskites (0D), Cs4PbBr6 and Cs4PbI6, through a comparative analysis between 0D and three-dimensional (3D) perovskites. A series of optical studies excluded the 3D phases as the origin of emission in these materials. In parallel, the results from the DFT proposed the defects as a possible origin of emission. The second part of the thesis addresses the shortcoming of lead-based perovskites in terms of toxicity and stability, motivated by the high demand for sustainable materials with analogous electrical and structural properties. Thus, a series of solid-state Zn-based and Mn-based ternary compounds were investigated with and without doping. The compounds' photoluminescence peaks were between 520 nm – 525 nm, with PLQY between 34% -60%. Finally, CsMnBr3 NCs were synthesized revealing an intense red PL peak centered at 650 nm and a PLQY as high as 54% along with a remarkable excitation spectrum and surprisingly short lifetimes. The single crystals of this composition were also reported with a PL peak at 640 nm and a relatively high PLQY of 6.7% under the excitation at 360 nm. Further, a combination of structural and optical analysis attributed the green and red luminescence to the tetrahedral and octahedral environment of Mn2+, respectively. These materials represent a milestone towards lead-free luminescent materials with interesting optical properties. This dissertation aims at engineering different materials to address critical aspects in the field including stability and good luminescence properties while simultaneously examining the photophysics and mechanisms of the corresponding properties. This work paves the way for finding sustainable light-emitting materials for the next generation of light-emitting applications.
Date of AwardOct 27 2020
Original languageEnglish (US)
Awarding Institution
  • Physical Science and Engineering
SupervisorOsman Bakr (Supervisor)

Keywords

  • Lead-Free
  • Zero-Dimensioanl
  • Perovskites
  • PLQY
  • Luminescence
  • Manganese

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