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Perovskite light emitting diodes suffer from poor operational stability, exhibiting a rapid decay of external quantum efficiency within minutes to hours after turn-on. To address this issue, we explore surface treatment of perovskite films with phenylalkylammonium iodide molecules of varying alkyl chain lengths. Combining experimental characterization and theoretical modelling, we show that these molecules stabilize the perovskite through suppression of iodide ion migration. The stabilization effect is enhanced with increasing chain length due to the stronger binding of the molecules with the perovskite surface, as well as the increased steric hindrance to reconfiguration for accommodating ion migration. The passivation also reduces the surface defects, resulting in a high radiance and delayed roll-off of external quantum efficiency. Using the optimized passivation molecule, phenylpropylammonium iodide, we achieve devices with an efficiency of 17.5%, a radiance of 1282.8 W sr−1 m−2 and a record T50 half-lifetime of 130 h under 100 mA cm−2., Perovskite light emitting diodes suffer from operational stability, showing rapid decay of performance within minutes to hours after turn-on. Here, the authors investigate how the steric and Coulomb interaction of ammonium passivation molecules with varying alkyl chain length can improve device stability by suppressing iodide ion migration.

Perovskite light-emitting diodes (PeLEDs) have recently shown significant progress with external quantum efficiencies (EQEs) exceeding 20%. However, PeLEDs with pure-red (620-660 nm) light emission, an essential part for full-color displays, remain a great challenge. Herein, a general approach of spacer cation alloying is employed in Ruddlesden-Popper perovskites (RPPs) for efficient red PeLEDs with precisely tunable wavelengths. By simply tuning the alloying ratio of dual spacer cations, the thickness distribution of quantum wells in the RPP films can be precisely modulated without deteriorating their charge-transport ability and energy funneling processes. Consequently, efficient PeLEDs with tunable emissions between pure red (626 nm) and deep red (671 nm) are achieved with peak EQEs up to 11.5%, representing the highest values among RPP-based pure-red PeLEDs. This work opens a new route for color tuning, which will spur future developments of pure-red or even pure-blue PeLEDs with high performance. Ministry of Education (MOE) National Research Foundation (NRF) Published version This work was financially supported by the ERC Starting Grant (No. 717026), the Swedish Research Council VR (No. 2018–07109), the Swedish Foundation for International Cooperation in Research and Higher Education (No. CH2018-7736), and the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO-Mat-LiU no. 2009-00971). The computational work for this article was fully performed on resources of the National Supercomputing Centre (NSCC), Singapore (https://www.nscc.sg). S.R., Q.X., X.-K.L., and T.C.S. acknowledge the support from Nanyang Technological University under its start-up grant (M4080514); the Ministry of Education, Singapore, under its AcRF Tier 2 grants (MOE2019-T2-1-006 and MOE-T2EP50120-0004); and the National Research Foundation (NRF), Singapore, under its NRF Investigatorship (NRF-NRFI2018-04). L.H. thanks the NSFC Project (61774077), the Key Projects of Joint Fund of Basic and Applied Basic Research Fund of Guangdong Province (2019B1515120073, 2019B090921002, 2020A1414010036), and the Guangzhou Key laboratory of Vacuum Coating Technologies and New Energy Materials Open Projects Fund (KFVE20200006) for financial support. Z.C. thanks the project funded by China Postdoctoral Science Foundation (2020M673055). J.Q. acknowledges the support by the Science and Technology Planning Project of Guangzhou, China (Grant No. 201605030008), and the Fundamental Research Funds for the Central Universities (Grant No. 21621008)

Perovskite light-emitting diodes (PeLEDs) have experienced rapid improvements in device efficiency during the last several years. However, the operational instability of PeLEDs remains a key barrier hindering their practical applications. A fundamental understanding of the degradation mechanism is still lacking but will be important to seek ways to mitigate these unwanted processes. In this work, through comprehensive characterizations of the perovskite emitters and the interfacial contacts, we figure out that Joule heating induced interface degradation is one of the dominant factors affecting the operational stability of PeLEDs. We investigate the interfacial contacts of PeLEDs based on a commonly used device structure, with an organic electron transport layer of 1,3,5-tris(N-phenylbenzimiazole-2-yl)benzene (TPBi), and observe obvious photoluminescence quenching of the perovskite layer after device operation. Detailed characterizations of the interlayers and the interfacial contacts reveal that photoluminescence quenching is mainly due to the element inter-diffusion at the interface induced by the morphological evolution of the TPBi layers under Joule heating during the operation of PeLEDs. Our work provides direct insights into the degradation pathways and highlights the importance of exploring intrinsically stable interlayers as well as interfacial contacts beyond the state-of-the-art to further boost the operational stability of PeLEDs. Funding Agencies|National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [91833303, 61974098, 61674108]; National Key Research and Development Program [2016YFA0201900]; Priority Academic Program Development of Jiangsu Higher Education Institutions; 111 programMinistry of Education, China - 111 Project; Collaborative Innovation Center of Suzhou Nano Science and Technology (NANO-CIC); ERC Starting GrantEuropean Research Council (ERC) [717026]; Swedish Energy Agency EnergimyndighetenSwedish Energy Agency [48758-1]; Swiss National Science Foundation (SNF)-Bridge POWERSwiss National Science Foundation (SNSF) [20B2-1_176552/1]; Postgraduate Research & Practice Innovation Program of Jiangsu Province [KYCX18_2504]; China Scholarship CouncilChina Scholarship Council [201806920071]

Metal halide perovskites are promising materials for the fabrication of cost-effective and highperformance light-emitting diodes (LEDs), due to their solution processability, high photoluminescence ...

Room-temperature spin-based electronics is the vision of spintronics. Presently, there are few suitable material systems. Herein, we reveal that solution-processed mixed-phase Ruddlesden–Popper perovskite thin-films transcend the challenges of phonon momentum-scattering that limits spin-transfer in conventional semiconductors. This highly disordered system exhibits a remarkable efficient ultrafast funneling of photoexcited spin-polarized excitons from two-dimensional (2D) to three-dimensional (3D) phases at room temperature. We attribute this efficient exciton relaxation pathway towards the lower energy states to originate from the energy transfer mediated by intermediate states. This process bypasses the omnipresent phonon momentum-scattering in typical semiconductors with stringent band dispersion, which causes the loss of spin information during thermalization. Film engineering using graded 2D/3D perovskites allows unidirectional out-of-plane spin-funneling over a thickness of ~600 nm. Our findings reveal an intriguing family of solution-processed perovskites with extraordinary spin-preserving energy transport properties that could reinvigorate the concepts of spin-information transfer., Spin-information transport or transfer is essential for spintronics applications and often relies on high purity and quality materials. Here, the authors report on the defect-tolerant solution-processed Ruddlesden–Popper halide perovskites, where a spin propagation length of 600 nm was achieved via spin funneling.

Semiconductor quantum dots (QDs) are among the most promising next-generation optoelectronic materials. QDs are generally obtained through either epitaxial or colloidal growth and carry the promise for solution-processed high-performance optoelectronic devices such as light-emitting diodes (LEDs), solar cells, etc. Herein, a straightforward approach to synthesize perovskite QDs and demonstrate their applications in efficient LEDs is reported. The perovskite QDs with controllable crystal sizes and properties are in situ synthesized through one-step spin-coating from perovskite precursor solutions followed by thermal annealing. These perovskite QDs feature size-dependent quantum confinement effect (with readily tunable emissions) and radiative monomolecular recombination. Despite the substantial structural inhomogeneity, the in situ generated perovskite QDs films emit narrow-bandwidth emission and high color stability due to efficient energy transfer between nanostructures that sweeps away the unfavorable disorder effects. Based on these materials, efficient LEDs with external quantum efficiencies up to 11.0% are realized. This makes the technologically appealing in situ approach promising for further development of state-of-the-art LED systems and other optoelectronic devices. Funding Agencies|ERC Starting Grant [717026]; Carl Tryggers Stiftelse; European Commission Marie SklodowskaCurie Actions [691210]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009-00971]; China Scholarship Council

Metal halide perovskite nanocrystals (NCs) have demonstrated great advances for light-emitting diodes (LEDs) applications, owing to their excellent optical, electrical properties and cost-effective solution-processing potentials. Tremendous progress has been made in perovskite NCs-based LEDs during the past several years, with the external quantum efficiency (EQE) boosted to over 20 %. Recently, metal doping/alloying strategy has been explored to finely tune the optoelectronic properties and enhance material stability of perovskite NCs, leading to further improved device efficiency and stability of the obtained perovskite NCs-based LEDs. In this review, we summarize recent progress on the metal doping/alloying of perovskite NCs and their applications in LEDs. We focus on the effects of different metal doping strategies on the structural and optoelectronic properties of the perovskite NCs. In addition, several works on high-performance LEDs based on metal doped/alloyed perovskite NCs with different light emission colours are highlighted. Finally, we present an outlook on employing metal doping/alloying strategies to further improve the device efficiency and stability of LEDs based on perovskite NCs.

Herein, an insulating biopolymer is exploited to guide the controlled formation of micro/nano-structure and physical confinement of alpha-delta mixed phase crystalline grains of formamidinium lead iodide (FAPbI(3)) perovskite, functioning as charge carrier concentrators and ensuring improved radiative recombination and photoluminescence quantum yield (PLQY). This composite material is used to build highly efficient near-infrared (NIR) FAPbI(3) Perovskite light-emitting diodes (PeLEDs) that exhibit a high radiance of 206.7 W/sr*m(2), among the highest reported for NIR-PeLEDs, obtained at a very high current density of 1000 mA/cm(2), while importantly avoiding the efficiency roll-off effect. In depth photophysical characterization allows to identify the possible role of the biopolymer in i) enhancing the radiative recombination coefficient, improving light extraction by reducing the refractive index, or ii) enhancing the effective optical absorption because of dielectric scattering at the polymer-perovskite interfaces. Our study reveals how the use of insulating matrixes for the growth of perovskites represents a step towards high power applications of PeLEDs. Funding Agencies|Regione Puglia through Samset2018 [r_puglia/A00_137/PROT/17/07/2017/001578]; MIUR (Italian Ministry of University and Research) through PRIN PERovskite-based Solar cells: towards high Efficiency and lOng-term stability (PERSEO) [20155LECAJ]; Fondazione di Sardegna - Convenzione triennale tra la Fondazione di Sardegna e gli Atenei Sardi Regione Sardegna [L.R. 7/2007, F72F16003040002]; SIR project "Two-Dimensional Colloidal Metal Dichalcogenides based Energy-Conversion Photovoltaics" (2D ECO), Bando SIR (Scientific Independence of young Researchers) 2014 MIUR Decreto Direttoriale 23 gennaio 2014 [197, RBSI14FYVD, CUP: B82I15000950008]; Regione Puglia; ARTI [LSBC6N4, GOWMB21]; China Scholarship Council

Chemical doping is often used to enhance electric conductivity of the conjugated molecule as hole-transporting material (HTM) for the application in optoelectronics. However, chemical dopants can promote ion migration at the electrical field, which deteriorates the device efficiency as well as increases the fabrication cost. Here, two star HTMs, namely 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenyl-amine) 9,9′-spirobifluorene (Spiro-OMeTAD) and poly(triarylamine) are subjeted to chemical combination to yield dopant-free N2,N2,N2′,N2′,N7,N7,N7′,N7′-octakis(4-methoxyphenyl)-10-phenyl-10H-spiro[acridine-9,9′-fluorene]-2,2′,7,7′-tetraamine (SAF-OMe). The power conversion efficiencies (PCEs) of 12.39% achieved by solar cells based on pristine, dopant-free SAF-OMe are among the highest reported for perovskite solar cells and are even comparable to devices based on chemically doped Spiro-OMeTAD (14.84%). Moreover, using a HTM comprised of SAF-OMe with an additional dopant results in a record PCE of 16.73%. Compared to Spiro-OMeTAD-based devices, SAF-OMe significantly improves stability.

Layered bismuth selenide (L-Bi2Se3) nanoplates were implemented as hole transporting layers (HTLs) for inverted organic solar cells. Device based on L-Bi2Se3 showed increasing power conversion efficiency (PCE) during ambient condition storage process. A PCE of 4.37% was finally obtained after 5 days storage, which outperformed the ones with evaporated-MoO3 using poly(3-hexylthiophene) (P3HT) as donor material and [6,6]-phenyl-C61-butyric acid methyl ester (PC61BM) as acceptor. The improved device efficiency can be attributed to the high conductivity and increasing work function of L-Bi2Se3. The work function of L-Bi2Se3 increased with the storage time in ambient condition due to the oxygen atom doping. Ultraviolet photoelectron spectroscopy and high resolution X-ray photoelectron spectroscopy were conducted to verify the increased work function, which originated from the p-type doping process. The device based on L-Bi2Se3 exhibited excellent stability in ambient condition up to 4 months, which was much improved compared to the device based on traditional HTLs.

Light-emitting diodes (LEDs) based on organic-inorganic hybrid perovskites, in particular, 3D and quasi-2D ones, are in the fast development and their external quantum efficiencies (EQEs) have exceeded 10%, making them competitive candidates toward large-area and low-cost light-emitting applications allowing printing techniques. Similar to other LED categories, light out-coupling efficiency is an important parameter determining the EQE of perovskite LEDs (PeLEDs), which, however, is scarcely studied, limiting further efficiency improvement and understanding of PeLEDs. In this work, for the first time, optical energy losses in PeLEDs are investigated through systematic optical simulations, which reveal that the 3D and quasi-2D PeLEDs can achieve theoretically maximum EQEs of approximate to 25% and approximate to 20%, respectively, in spite of their high refractive indices. These results are consistent with the reported experimental data. This work presents primary understanding of the optical energy losses in PeLEDs and will spur new developments in the aspects of device engineering and light extraction techniques to boost the EQEs of PeLEDs. Funding Agencies|ERC [717026]; Carl Tryggers Stiftelse; European Commission [691210]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009-00971]; National Basic Research Program of China [2016YFE0112000]; European Union [2016YFE0112000]; State Key Laboratory of Luminescent Materials and Devices at South China University of Technology [2017-skllmd-05]; State Key Lab of Silicon Materials at Zhejiang University [SKL2017-03]; China Scholarship Council [201506920047]; [2016-02051]

Solution-processed tin dioxide is employed as an electron transport layer in n–i–p-structured perovskite light-emitting diodes realizing an EQE of 7.9%., To achieve high-performance perovskite light-emitting diodes (PeLEDs), an appropriate functional layer beneath the perovskite emissive layer is significantly important to modulate the morphology of the perovskite film and to facilitate charge injection and transport in the device. Herein, for the first time, we report efficient n–i–p structured PeLEDs using solution-processed SnO2 as an electron transport layer. Three-dimensional perovskites, such as CH(NH2)2PbI3 and CH3NH3PbI3, are found to be more chemically compatible with SnO2 than with commonly used ZnO. In addition, SnO2 shows good transparency, excellent morphology and suitable energy levels. These properties make SnO2 a promising candidate in both three- and low-dimensional PeLEDs, among which a high external quantum efficiency of 7.9% has been realized. Furthermore, interfacial materials that are widely used to improve the device performances of ZnO-based PeLEDs are also applied on SnO2-based PeLEDs and their effects have been systematically studied. In contrast to ZnO, SnO2 modified by these interfacial materials shows detrimental effects due to photoluminescence quenching.

Graphene oxide (GO) is employed as a hole conductor in inverted planar heterojunction perovskite solar cells, and the devices with CH₃NH₃PbI₃-xClx as absorber achieve an efficiency of over 12%. The perovskite film grown on GO exhibits enhanced crystallization, high surface coverage ratio as well as preferred in-plane orientation of the (110) plane. Efficient hole extraction from the perovskite to GO is demonstrated.

Solar cell generates electrical energy from light one via pulling excited carrier away under built-in asymmetry. Doped semiconductor with antireflection layer is general strategy to achieve this including crystalline silicon (c-Si) solar cell. However, loss of extra energy beyond band gap and light reflection in particular wavelength range is known to hinder the efficiency of c-Si cell. Here, it is found that part of short wavelength sunlight can be converted into polarization electrical field, which strengthens asymmetry in organic-c-Si heterojunction solar cell through molecule alignment process. The light harvested by organometal trihalide perovskite nanoparticles (NPs) induces molecular alignment on a conducting polymer, which generates positive electrical surface field. Furthermore, a "field-effect solar cell" is successfully developed and implemented by combining perovskite NPs with organic/c-Si heterojunction associating with light-induced molecule alignment, which achieves an efficiency of 14.3%. In comparison, the device with the analogous structure without perovskite NPs only exhibits an efficiency of 12.7%. This finding provides a novel concept to design solar cell by sacrificing part of sunlight to provide "extra" asymmetrical field continuously as to drive photogenerated carrier toward respective contacts under direct sunlight. Moreover, it also points out a method to combine promising perovskite material with c-Si solar cell.