CHAPTER 7. Summary
7.1. Summary
This thesis presents effective approaches to developing dimension-engineered quasi-2D blue emissive perovskite materials and overcoming the lagged efficiency of blue emissive PeLEDs. The inherent multiple-quantum well structure i.e., assembly of quasi-2D perovskite phases endows them with outstanding optical properties such as bandgap tunability, high exciton binding energy, and high PLQY under a low excitation intensity. Therefore, the modulation of 2D phases for efficient quasi-2D perovskite materials having an ideal energy landscape, optimal phase distribution, and favorable orientation, can realize efficient and stable blue PeLEDs.
In chapter 2, an effective interfacial engineering strategy was introduced to guide the formation of well-grown 2D perovskite phases and minimize the detrimental chemical damage from the highly acidic PEDOT:PSS substrate. Zwitterion additive, L-phenylalanine contains carboxylate and ammonium functionalities that buffer the acidity of PEDOT:PSS and are able to coordinate to uncoordinated Pb2+
in the overlying perovskite layer, was incorporated into the PEDOT:PSS. The bidentate coordination between additive and uncoordinated Pb2+ facilitates the growth of 2D perovskite phases and even thoroughly passivates the interfacial defect states. Moreover, attenuated acidity of the PEDOT:PSS suppresses the chemical etching of ITO substrates, reducing exciton quenching pathways. Finally, we realized efficient and stable sky-blue emissive PeLEDs with a peak EQE of 10.98% at 480 nm by blocking energy loss due to defect states through and designing an ideal energy landscape.
In chapter 3, a multifunctional passivating molecule of 36ClCzEPA, containing the electron- withdrawing chlorine atom and the phosphonic acid as a functional and anchoring group was introduced as an alternative to the highly acidic PEDOT:PSS HIL. It was observed that this molecule formed a SAM on the ITO substrate, altering the electronic structure of the ITO electrode with significantly increased WF. Strongly chemisorbed neutral SAM inhibited the chemical etching of ITO and perovskite emissive layer, leading to the suppression of exciton quenching pathways. Besides, the incorporated chlorine atom induced an orbital coupling with the interfacial uncoordinated Pb2+detect state as well as a strong interfacial dipole, passivating them and thereby resulting in a hypsochromically shifted optical properties of the perovskite layer. Finally, due to these synergetic effects originating from a well- designed SAM molecule, we realized efficient pure-blue emissive PeLEDs with a maximum luminance of 1253 cd m–2and a peak EQE of 4.80% at 473 nm.
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In chapter 4, the effect of the surface polarity of the underlying HIL on the crystallization dynamics of 2D perovskite phases was thoroughly studied, and optimized the surface polarity to realize the optimal substrate for efficient pure-blue emissive PeLEDs. Three different additives, L-phenylalanine, L-tyrosine, and L-dopa as surface-modifying agents were incorporated into the PEDOT:PSS. It was confirmed that the additive, L-dopa involving hydroxyl groups coordinate chemical bonding with the sulfonate group of PSS moieties, leading to a higher surface polarity for the PEDOT:PSS substrate. On that substrate, the formation of higher-n2D perovskite phases was thermodynamically unfavorable due to the smaller formation energy, and lower-n-dominated phase distribution induced a hypsochromically shift in the luminescence spectrum. Finally, to obtain the optimal substrate for efficient pure-blue emissive PeLEDs, we controlled the dual additives with L-phenylalanine which provide a well-matched electronic band structure, boosting the performance of pure-blue emissive PeLEDs with a maximum EQE of 5.57% at 472 nm.
In chapter 5, a facile halide and phase modulating approach to design an ideal energy-transfer tunnel structure with flawless quasi-2D perovskites was introduced. This post-treatment entails the halide- exchange reaction with the assistance of haloalkane molecules and strong nucleophile molecules. The detached chlorides from the haloalkane molecule spontaneously exchanged with bromides in perovskites and further intrude the chlorine vacant sites, resulting in efficient PL and color stability.
Furthermore, the spontaneous phase rearrangement occurred via merging between neighboring low-n 2D phases to higher-n2D phases. It modulated the landscape of the energy-transfer funnel to have the narrowed 2D phase distribution, minimizing the detrimental exciton losses through the streamlined energy transfer. Finally, we realized efficient deep-blue emissive PeLEDs with a maximum EQE of 4.97% at 470 nm due to all synergetic effects from the proposed halide and phase rearrange treatment.
In chapter 6, a facile halide post-treatment was also introduced to realize efficient bulk blue emissive perovskite films. The halide compositions of bulk perovskite films were finely controlled for the desired emission colors. This spontaneous halide exchange process induced the recrystallization of rough perovskite surface, providing a fully covered and smooth perovskite film. Finally, we realized highly luminescent blue emissive bulk PeLEDs with maximum luminance of 1468 and 495 cd m–2at 490 and 470 nm, respectively. Also, this post-treatment resulted in long operating lifetimes of 7.74 and 3.06 min under a high-level of current injection (~20 mA cm–2) without halide segregation.
Overall, we systemically introduced quasi-2D perovskite materials and developed strategic approaches for realizing efficient and stable blue PeLEDs. Since most of the outstanding optical and photophysical properties of quasi-2D perovskite materials could be determined by the assembly of 2D perovskite phases, the modulation of 2D phases is essential for idealized blue emissive quasi-2D perovskite materials and their device applications. Our suggested approaches, we believe, would provide a versatile avenue to improving the efficiency of blue PeLEDs, bringing the field a step closer to practical and commercial applications.
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