Defect Passivation and Surface Modification for Efficient and Stable Organic-Inorganic Hybrid Perovskite Solar Cells and Light-Emitting Diodes

Abstract

Defect passivation and surface modification of perovskite semiconductors play a key role in achieving highly efficient and stable perovskite solar cells (PSCs) and light-emitting diodes (LEDs). This dissertation describes three novel strategies for such defect passivation and surface modification. In the first strategy, we demonstrate a facile approach using inorganic perovskite quantum dots (QDs) to supply bulk- and surface-passivation agents to combine high power conversion efficiency (PCE) with high stability in CH3NH3PbI3 (MAPbI3) inverted PSCs. This strategy utilizes inorganic perovskite QDs to distribute elemental dopants uniformly across the MAPbI3 film and attach ligands to the film’s surface. Compared with pristine MAPbI3 films, MAPbI3 films processed with QDs show a reduction in tail states, smaller trap-state density, and an increase in carrier recombination lifetime. The strategy results in reduced voltage losses and an improvement in PCE from 18.3% to 21.5%, which is among the highest efficiencies for MAPbI3 devices. The devices maintain 80% of their initial PCE under 1-sun continuous illumination for 500 h and show improved thermal stability. In the second strategy, we reduce the efficiency gap between the inverted PSCs and regular PSCs using a trace amount of surface-anchoring, long-chain alkylamine ligands (AALs) as grain and interface modifiers. We show that long-chain AALs suppress nonradiative carrier recombination and improve the optoelectronic properties of mixed-cation mixed-halide perovskite films. These translate into a certified stabilized PCE of 22.3% (23.0% PCE for lab-measured champion devices). The devices operate for over 1000 hours at the maximum power point (MPP), under simulated AM1.5 illumination, without loss of efficiency. Finally, we report a strategy to passivate Cl vacancies in mixed halide perovskite (MHP) QDs using non-polar-solvent-soluble organic pseudohalide (n-dodecylammonium thiocyanate (DAT)), enabling blue MHP LEDs with enhanced efficiency. Density-function-theory calculations reveal that the thiocyanate (SCN-) groups fill in the Cl vacancies and remove deep electron traps within the bandgap. DAT-treated CsPb(BrxCl1-x)3 QDs exhibit near unity (~100%) photoluminescence quantum yields; and their blue (~470 nm) LEDs are spectrally stable with an external quantum efficiency (EQE) of 6.3% – a record for perovskite LEDs emitting at the 460-480 nm range relevant to Rec. 2020 display standards.

Date of Award	Feb 26 2020
Original language	English (US)
Awarding Institution	Physical Sciences and Engineering
Supervisor	Osman Bakr (Supervisor)