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Charge-transfer excitons (CTEs) immensely enrich property-tuning capabilities of semiconducting materials. However, such concept has been remaining as unexplored topic within halide perovskite structures. Here, we report that CTEs can be effectively formed in heterostructured 2D perovskites prepared by mixing PEA2PbI4:PEA2SnI4, functioning as host and guest components. Remarkably, a broad emission can be demonstrated with quick formation of 3 ps but prolonged lifetime of ~0.5 μs. This broad PL presents the hypothesis of CTEs, verified by the exclusion of lattice distortion and doping effects through demonstrating double-layered PEA2PbI4/PEA2SnI4 heterostructure when shearing-away PEA2SnI4 film onto the surface of PEA2PbI4 film by using hand-finger pressing method. The below-bandgap photocurrent indicates that CTEs are vital states formed at PEA2PbI4:PEA2SnI4 interfaces in 2D perovskite heterostructures. Electroluminescence shows that CTEs can be directly formed with electrically injected carriers in perovskite LEDs. Clearly, the CTEs presents a new mechanism to advance the multifunctionalities in 2D perovskites.

A kind of sandwich-like NiCo2O4/rGO/NiO heterostructure composite has been successfully anchored on nickel foam substrate via a three-step hydrothermal method with successive annealing treatment. The smart combination of NiCo2O4, reduced graphene oxide (rGO), and NiO nanostructure in the sandwich-like nano architecture shows a promising synergistic effect for supercapacitors with greatly enhanced electrochemical performance. For serving as supercapacitor electrode, the NiCo2O4/rGO/NiO heterostructure materials exhibit remarkable specific capacitance of 2644 mF cm−2 at current density of 1 mA cm−2, and excellent capacitance retentions of 97.5% after 3000 cycles. It is expected that the present heterostructure will be a promising electrode material for high-performance supercapacitors.Graphical Abstract

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This paper reports a new method to generate stable and high-brightness electroluminescence (EL) by subsequently growing large/small grains at micro/nano scales with the configuration of attaching small grains on the surfaces of large grains in perovskite (MAPbBr 3) films by mixing two precursor solutions (PbBr 2 + MABr and Pb(Ac) 2 $3H 2 O + MABr). Consequently, the small and large grains serve, respectively, as passivation agents and light-emitting centers, enabling self-passivation on the defects located on the surfaces of light-emitting large grains. Furthermore, the light-emitting states become linearly polarized with maximal polarization of 30.8%, demonstrating a very stable light emission (49,119 cd/m 2 with EQE = 11.31%) and a lower turn-on bias (1.9 V) than the bandgap (2.25V) in the perovskite LEDs (ITO/PEDOT:PSS/MAPbBr 3 /TPBi[50 nm]/LiF[0.7 nm]/Ag). Therefore, mixing large/ small grains with the configuration of attaching small grains on the surfaces of large grains by mixing two precursor solutions presents a new strategy to develop high-performance perovskite LEDs.

Excited states in organic light-emitting diodes (OLEDs) are inevitably formed with both singlets and triplets under electrical excitation. Singlets and triplets are allowed and forbidden to recombine, respectively, due to spin selection rule. It has been shown that the triplets can be almost 100% converted into singlets in thermally activated delayed fluorescence (TADF) molecules based on the design of chemically combining donor and acceptor moieties to enable intramolecular chargetransfer states. [1][2][3][4] Recently, various TADFmolecule-based OLEDs with extremely high external quantum efficiency (EQE) exceeding 35% have been successfully demonstrated. [5,6] Similarly, high EQEs can also be conveniently realized by physically mixing donor and acceptor components to form intermolecular charge-transfer states in exciplex systems, where the nonradiative triplets are also largely converted into radiative singlets. The advantages and versatile applications of exciplex systems for giving high-efficiency OLEDs have been highlighted recently. [7] More significantly, OLEDs with exciplex-forming systems as emitting layer have been reported to achieve EQE higher than 19%, [8][9][10] manifesting their bright and promising prospects in OLED technology based on physically Experimental studies to reveal the cooperative relationship between spin, energy, and polarization through intermolecular charge-transfer dipoles to harvest nonradiative triplets into radiative singlets in exciplex lightemitting diodes are reported. Magneto-photoluminescence studies reveal that the triplet-to-singlet conversion in exciplexes involves an artificially generated spin-orbital coupling (SOC). The photoinduced electron parametric resonance measurements indicate that the intermolecular charge-transfer occurs with forming electric dipoles (D +• →A −• ), providing the ionic polarization to generate SOC in exciplexes. By having different singlet-triplet energy differences (ΔE ST ) in 9,9′-diphenyl-9H,9′H-3,3′-bicarbazole (BCzPh):3′,3′″,3′″″-(1,3,5-triazine-2,4,6-triyl) tris(([1,1′-biphenyl]-3-carbonitrile)) (CN-T2T) (ΔE ST = 30 meV) andBCzPh:bis-4,6-(3,5-di-3-pyridylphenyl)-2-methyl-pyrimidine (B3PYMPM) (ΔE ST = 130 meV) exciplexes, the SOC generated by the intermolecular charge-transfer states shows large and small values (reflected by different internal magnetic parameters: 274 vs 17 mT) with high and low external quantum efficiency maximum, EQE max (21.05% vs 4.89%), respectively. To further explore the cooperative relationship of spin, energy, and polarization parameters, different photoluminescence wavelengths are selected to concurrently change SOC, ΔE ST , and polarization while monitoring delayed fluorescence. When the electron clouds become more deformed at a longer emitting wavelength due to reduced dipole (D +• →A −• ) size, enhanced SOC, increased orbital polarization, and decreased ΔE ST can simultaneously occur to cooperatively operate the triplet-to-singlet conversion.

This paper reports our experimental studies on the underlying mechanism responsible for electroluminescence spectral narrowing phenomenon in the cavity-based organic light-emitting diodes. It is found that the microcavity generates an emerging phenomenon: a magneto-photoluminescence signal in Poly(9,9-dioctylfluorene-alt-benzothiadiazole) polymer under photoexcitation, which is completely absent when microcavity is not used. This provides an evidence that microcavity leads to the formation of spatially extended states, functioning as the intermediate states prior to the formation of Frenkel excitons in organic materials. This is confirmed by the magneto-electroluminescence solely observed from the cavity-based light-emitting diodes under electrical injection. Furthermore, the narrowed electroluminescence output shows a linear polarization, concurrently occurred with magneto-electroluminescence. This indicates that the spatially extended sates become aligned towards forming coherent light-emitting excitons within the microcavity through optical resonance. Clearly, the spatially extended states present the necessary condition to realize electroluminescence spectral narrowing phenomenon towards lasing actions in cavity-based organic light-emitting diodes.

Given the remarkable performance of hybrid organic–inorganic perovskites (HOIPs) in solar cells, light emitters, and photodetectors, the quest to advance the fundamental understanding of the photophysical properties in this class of materials remains highly relevant. Recently, the discovery of ferroic twin domains in HOIPs has renewed the debate of the ferroic effects on optoelectric processes. This work explores the interaction between light and ferroic twin domains in CH3NH3PbI3. Due to strain and chemical inhomogeneities, photogenerated electrons and holes show a preferential motion in the ferroelastic twin domains. Density functional theory (DFT) shows that electrons and holes result in lattice expansion in CH3NH3PbI3 differently. Hence, light generates strain in the ferroelastic domains due to preferential photocarrier motion, leading to a screening of strain variation. X‐ray diffraction studies verify the DFT simulations and reveal that the photoinduced strain is light intensity dependent, and the photoexcitation is a prerequisite of inducing strain by light. This work extends the fundamental understanding of light‐ferroic interaction and offers guidance for developing functional devices.