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Metal halide perovskites have attracted significant attention for light-emitting applications, because of their excellent properties, such as high photoluminescence quantum yields (PLQYs), good charge mobility, narrow emission bandwidth, readily tunable emission spectra ranging from ultraviolet to near-infrared, and solution processability. Since the first room-temperature perovskite-based light-emitting diodes (PeLEDs) reported in 2014, tremendous efforts have been made to promote the efficiencies of PeLEDs, including theoretical simulation, materials design, and device engineering. To reach the ultimate goal of commercialization, PeLEDs with both high-efficiency and long-term operational stability are desired. Achieving high-quality perovskite emissive films is key towards this goal. Centering around the high-quality perovskite films, in this thesis, we demonstrate effective synthesis strategies for the deposition of high-quality perovskite films (including both three-dimensional and mixed-dimensional perovskites) and investigate the effects of ion migration in the perovskite films on the performance of PeLEDs. Due to the fast crystallization nature of perovskites and the low formation energy of defects, controlling the crystallization processes of these films has proved to be an effective approach for achieving high-quality perovskite films. For three-dimensional (3D) perovskite films, we have controlled the formation of these films through the assistance of molecules with the amino group. Herein, we have chosen an electron-transport molecule with two amino groups, 4,4’-diaminodiphenyl sulfone (DDS), to control the crystallization process of perovskite films (Paper 1). The resulting perovskite films consists of in-situ formed high quality perovskite nanocrystals embedded in the electron-transport molecular matrix, resulting in improved PLQYs and structural stability. PeLEDs based on these perovskite films have exhibited both high efficiency and long operational stability. In addition, we have investigated the formation of mixed-dimensional perovskite films. Efficient PeLEDs based on mixed-dimensional perovskite films were fabricated with tin dioxide (SnO2) as an electron transport layer (Paper 3). We also note that the deposition methods have a significant impact on the morphology and optical properties of prepared mixed-dimensional perovskite films (Paper 4). In addition, we provide an effective method to extend the deposition of mixed-dimensional perovskite films, replacing organic ammonium halides with amines in the perovskite precursor solutions to form organic spacer cations through the in-situ protonation process of amines (Paper 2). In spite of these efforts, the performance of PeLEDs is still far from the commercialization standard, partially limited by ion migration. In Paper 5, we discuss impacts of mobile ions in the perovskite films on the performance of PeLEDs. We find that a dynamic redistribution of mobile ions can change current density of a device, leading to EQE/hysteresis during forward and reverse voltage scan and enhanced EQE under constant driving voltages. In addition, we have found that excess mobile ions in the perovskite layer can aggravate the hysteresis and shorten the operational stability of PeLEDs. In this thesis, we also discuss the remaining key challenges in the PeLED field, including the achievement of high-performance blue, white, and lead-free PeLEDs, as well as possible strategies to address these challenges. We hope that our research findings provide insights into the basic science behind the perovskite materials, and broadly benefit other optoelectronic communities, such as perovskite solar cells, flexible electronics, and so on. Metall-halid-perovskiter har fått mycket uppmärksamhet för deras möjlighet att användas i ljusemitterande applikationer på grund utav utmärkta egenskaper så som högt fotoluminiscent kvantutbyte (PLQYs), god mobilitet, smalt emissionsband, lättjusterat emissionsspektra i intervallet ultraviolett till nära infrarött, samt för att de kan beredas med en lösningsbaserad process. Ända sedan de första perovskitbaserade ljusdioderna (PeLEDs) som verkande i rumstemperatur rapporterades 2014 har enormt arbete lagts ner på att öka effektiviteten hos PeLEDs, till exempel genom teoretiska simuleringar, materialdesign och teknisk utformning utav lysdioden. För att nå det slutgiltiga målet med kommersialisering behövs PeLEDs som har både hög effektivitet och driftstabilitet. Att uppnå högkvalitativa emitterande perovskitfilmer är nyckeln för att nå detta mål. I den här avhandlingen, vilken fokuserar på högkvalitativa perovskitfilmer, demonstrerar vi effektiva syntetiseringsstrategier för deponering utav högkvalitativa perovskitfilmer och undersöker effekterna jonmigration har på prestandan i perovskitfilmerna i PeLEDs. På grund utav den snabbkristalliserande naturen hos perovskitfilmer och den låga bildningsenergin för defekter så har kontroll utav kristallisationsprocessen av dessa filmer visat sig vara en effektiv väg för att uppnå högkvalitativa perovskitfilmer. När det gäller tredimensionella perovskitfilmer så har vi kontrollerat bildandet av dessa filmer genom assistans från molekyler med aminogrupper. Vi har valt en elektrontransporterande molekyl som har två aminogrupper, 4,4’- diaminodifenyl sulfon (DDS), för att kontrollera kristallisationsprocessen av perovskitfilmer (artikel 1). De beredda perovskitfilmerna bestod av insitu- bildade högkvalitativa perovskitnanokristaller inbäddade i en elektrontransporterande molekylär matris vilket resulterade i förbättrat fotoluminiscent-kvantutbyte och strukturell stabilitet. PeLEDs baserade på dessa perovskitfilmer har uppvisat både hög effektivitet och lång driftstabilitet. Därtill har vi undersökt bildandet av blanddimensionella perovskiter. Effektiva PeLEDs baserade på blanddimensionella perovskiter var tillverkade med tenndioxid (SnO2) som elektrontransportlager (artikel 3). Vi noterade även att val av deponeringsmetod hade signifikant effekt på IV morfologi och optiska egenskaper av de beredda blanddimensionella perovskitfilmerna (artikel 4). Därutöver tillhandahöll vi en effektiv metod för att deponera blanddimensionella perovskitfilmer genom att ersätta de vanligen använda organiska ammoniumhaliderna med aminer i prekursorlösningen för att bilda organiska distansierande katjonfilmer genom en in-situ-protoneringsprocess av aminer (artikel 2). Även om PeLEDs med högkvalitativa perovskitfilmer har visat förbättrad effektivitet och driftstabilitet så uppvisar lysdioderna fortfarande egenskaper som associeras med jonmigration. I artikel 5 diskuterar vi effekten av mobila joner i perovskitfilmer och hur de påverkar PeLEDs prestanda. Vi fann att den dynamiska omfördelningen av mobila joner i perovskitskiktet kan ändra det elektriska nettofältet i perovskitskiktet, modifiera laddningsbärarnas rekombination i perovskitskiktet och leda till ostadig strömdensitet. Dessutom har vi funnit att överskott av mobila joner i perovskitskiktet är en av de största anledningarna till den korta driftstabiliteten för PeLEDs. I denna avhandling diskuterar vi även kvarstående nyckelproblem i PeLED-fältet så som bedriften att uppnå högpresterande blå, vita och blyfria PeLEDs så väl som möjliga strategier att möta dessa utmaningar. Våra forskningsresultat ger insikter om den grundläggande vetenskapen bakom perovskitmaterialen vilka vi tror kommer vara till stort gagn för andra optoelektroniska fält, så som perovskitsolceller, flexibel elektronik och så vidare.

A major efficiency limit for solution-processed perovskite optoelectronic devices, for example light-emitting diodes, is trap-mediated non-radiative losses. Defect passivation using organic molecules has been identified as an attractive approach to tackle this issue. However, implementation of this approach has been hindered by a lack of deep understanding of how the molecular structures influence the effectiveness of passivation. We show that the so far largely ignored hydrogen bonds play a critical role in affecting the passivation. By weakening the hydrogen bonding between the passivating functional moieties and the organic cation featuring in the perovskite, we significantly enhance the interaction with defect sites and minimize non-radiative recombination losses. Consequently, we achieve exceptionally high-performance near-infrared perovskite light-emitting diodes with a record external quantum efficiency of 21.6%. In addition, our passivated perovskite light-emitting diodes maintain a high external quantum efficiency of 20.1% and a wall-plug efficiency of 11.0% at a high current density of 200 mA cm−2, making them more attractive than the most efficient organic and quantum-dot light-emitting diodes at high excitations. Funding agencies: ERC Starting Grant [717026]; National Basic Research Program of China (973 Program) [2015CB932200]; National Natural Science Foundation of China [61704077, 51572016, 51721001, 61634001, 61725502, 91733302, U1530401]; Natural Science Foundation of Jiangsu

Although perovskite light-emitting diodes (PeLEDs) have recently experienced significant progress, there are only scattered reports of PeLEDs with both high efficiency and long operational stability, calling for additional strategies to address this challenge. Here, we develop perovskite-molecule composite thin films for efficient and stable PeLEDs. The perovskite-molecule composite thin films consist of in-situ formed high-quality perovskite nanocrystals embedded in the electron-transport molecular matrix, which controls nucleation process of perovskites, leading to PeLEDs with a peak external quantum efficiency of 17.3% and half-lifetime of approximately 100 h. In addition, we find that the device degradation mechanism at high driving voltages is different from that at low driving voltages. This work provides an effective strategy and deep understanding for achieving efficient and stable PeLEDs from both material and device perspectives., The field of perovskite light-emitting diodes witnesses rapid development in both device processing strategies and performances. Here Wang et al. develop high-quality perovskite-molecule composite thin films and achieve high quantum efficiency of 17.3% and half-lifetime of 100 h.