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Stability is one of the major challenges in organic semiconductor based optoelectronic devices. A comparative study of thermally activated delayed fluorescence (TADF) based organic light emitting diodes (OLEDs) with alkali-halide lithium fluoride (LiF) vs alkaline halide magnesium fluoride (MgF2) inorganic electron injection interlayers is presented. A TADF emitter 4CzIPN doped in CBP is used as an active layer (thickness = 15 nm @6wt. % doping) in an OLED structure: Glass/ITO/PEDOT:PSS/NPD/CBP/CBP:4CzIPN/TPBi/interlayer/Al. Prior to this comparative study, a separate exercise is carried out to obtain an optimal thickness of an MgF2 interlayer on the basis of leakage current and efficiency in the TADF-OLEDs. OLEDs with an LiF interlayer showed an external quantum efficiency (EQE) of 19.7% in comparison with an MgF2 interlayer-based OLED showed slightly lower average EQE ∼19.1% at a luminance level of 100 cd/m2; these efficiency numbers are averaged over ∼60 OLEDs. These slight changes in EQE are supported by the relative photoluminescence quantum yield measurements with a whole device stack. However, alkaline halide MgF2 based TADF-OLEDs showed approximately seven-fold enhancement in the stability (LT60) under identical operating conditions. In situ photoluminescence monitoring of operational TADF-OLEDs confirmed that the probable cause of reduced lifetime is degradation of an LiF/TPBi interface. [ABSTRACT FROM AUTHOR]

The efficiency of an organic solar cell is highly dependent on the complex, interpenetrating morphology, and molecular order within the composite phases of the bulk heterojunction (BHJ) blend. Both these microstructural aspects are strongly influenced by the processing conditions and chemical design of donor/acceptor materials. To establish improved structure‐function relationships, it is vital to visualize the local microstructural order to provide specific local information about donor/acceptor interfaces and crystalline texture in BHJ blend films. The visualization of nanocrystallites, however, is difficult due to the complex semi‐crystalline structure with few characterization techniques capable of visualizing the molecular ordering of soft materials at the nanoscale. Here, it is demonstrated how cryo‐electron microscopy can be utilized to visualize local nanoscale order. This method is used to understand the distribution/orientation of crystallites in a BHJ blend. Long‐range (>300 nm) texturing of IEICO‐4F crystallites oriented in an edge‐on fashion is observed, which has not previously been observed for spin‐coated materials. This approach provides a wealth of quantitative information about the texture and size of nanocrystallites, which can be utilized to understand charge generation and transport in organic film. This study guides tailoring the material design and processing conditions for high‐performance organic optoelectronic devices. [ABSTRACT FROM AUTHOR]

Light emission from organoboron compounds of Schiff bases is found to depend strongly on their chemical structure. Two of these compounds (OB1 and OB2), which contain a benzene ring between the Schiff base moieties, exhibit weak fluorescence in methanol, with marked viscosity dependence. Fluorescence lifetimes of these compounds are in picosecond timescale, as determined by femtosecond optical gating (FOG). A significant enhancement in fluorescence intensity and lifetime is observed at 77 K, indicating the operation of an activated nonradiative process. Using fluorescence lifetime imaging microscopy (FLIM), OB1 and OB2 are shown to be potential membrane probes. The third (OB3), which is devoid of this benzene ring, exhibits relatively stronger fluorescence with nanosecond lifetimes at room temperature. No viscosity dependence is observed in this case. The emission spectrum at 77 K is markedly more intense and exhibits an additional red shifted structured feature, which persists for a few seconds. Hence, OB3 seems to have greater promise not only as fluorescent probe but also for light harvesting. The marked improvement of the light emission properties of OB3 compared with OB1 and OB2 is likely to serve as a pointer for the design of Schiff base‐derived organoboron luminophores with diverse potential applications. [ABSTRACT FROM AUTHOR]

Interface engineering is a critical parameter for optimal optoelectronic device performance. In quasi‐2D perovskite light emitting diodes (PeLEDs), traditional poly (3,4‐ethylene dioxythiophene) polystyrene sulfonate (PEDOT:PSS) hole injection layer (HIL) is replaced by self‐assembled monolayer (SAM) [2‐(3,6‐dibromo‐9H‐carbazol‐9‐yl) ethyl] phosphonic acid (Br‐2PACz) HIL. The deep highest occupied molecular orbital (HOMO @ −5.73 eV) of Br‐2PACz facilitates the efficient hole‐injection along with a reduction in leakage current by 4–5 orders of magnitude as compared to PEDOT:PSS (HOMO @ −5.00 eV) HIL based optimized PeLEDs. Ultra‐thin SAM‐based Br‐2PACz HIL presents two challenges: i) device reproducibility is hindered by spatial inhomogeneity, and ii) it fails to regulate nonradiative recombination at the perovskite/HIL interface. To address these challenges, the ultra‐thin interlayer of atomic layer deposited aluminum oxide (Al2O3) is utilized between Br‐2PACz, and perovskite which aids in passivating the interfacial states at the HIL/perovskite interface. With the optimized thickness of Al2O3 interlayer (3 nm), the device's external quantum efficiency (EQE) improved from 9.47% to 13.14%, accompanied by luminous efficiency of 42.8 cd A−1. An ultra‐thin interlayer of lithium fluoride (LiF) (2 nm) is implemented on the top side of the perovskite, which can provide 1.5 times increase in the device's LT50 stability. [ABSTRACT FROM AUTHOR]

Silver cluster‐based solids have garnered considerable attention owing to their tunable luminescence behavior. While surface modification has enabled the construction of stable silver clusters, controlling interactions among clusters at the molecular level has been challenging due to their tendency to aggregate. Judicious choice of stabilizing ligands becomes pivotal in crafting a desired assembly. However, detailed photophysical behavior as a function of their cluster packing remained unexplored. Here, we modulate the packing pattern of Ag12 clusters by varying the nitrogen‐based ligand. CAM‐1 formed through coordination of the tritopic linker molecule and NC‐1 with monodentate pyridine ligand; established via non‐covalent interactions. Both the assemblies show ligand‐to‐metal‐metal charge transfer (LMMCT) based cluster‐centered emission band(s). Temperature‐dependent photoluminescence spectra exhibit blue shifts at higher temperatures, which is attributed to the extent of the thermal reverse population of the S1 state from the closely spaced T1 state. The difference in the energy gap (ΔEST) dictated by their assemblies played a pivotal role in the way that Ag12 cluster assembly in CAM‐1 manifests a wider ΔEST and thus requires higher temperatures for reverse intersystem crossing (RISC) than assembly of NC‐1. Such assembly‐defined photoluminescence properties underscore the potential toolkit to design new cluster‐ assemblies with tailored optoelectronic properties. [ABSTRACT FROM AUTHOR]

Dark current is considered as one of the important parameters to suppress temporal noise and enhance sensitivity of photodetectors. This study shows the effect of active layer thickness and different interfacial layers in the suppression of leakage current. High-sensitivity (D* > 1012 Jones) perovskite photodetectors (PPDs) are fabricated using the device structure of ITO/PEDOT: PSS/FA0.95Cs0.05PbI3 (dPVSK)/ electron transport layer (ETL)/BCP/Ag with noise current <1 pA Hz−½. These PPDs have a broadband response from near-ultraviolet to near-infrared region (300–840 nm). The overall performance of the PPDs enhanced for the optimal thickness of active layer of dPVSK = 600 nm and ETL PC60BM layer thickness of dETL = 50 nm. The total noise current of the PPD is further suppressed by replacing the ETL PC60BM (in = 63.11 fA Hz−½) layer by a PC70BM (in = 33.41 fA Hz−½) layer. This further improved other figures of merit for these PPDs. Comparison with published reports on PPDs is included to compare with the state-of-the-art detectors. [ABSTRACT FROM AUTHOR]

Hybrid materials possessing piezo‐ and ferroelectric properties emerge as excellent alternatives to conventional piezoceramics due to their merits of facile synthesis, lightweight nature, ease of fabrication and mechanical flexibility. Inspired by the structural stability of aminophosphonium compounds, here we report the first A3BX6 type cyanometallate [Ph2(iPrNH)2P]3[Fe(CN)6] (1), which shows a ferroelectric saturation polarization (Ps) of 3.71 μC cm−2. Compound 1 exhibits a high electrostrictive coefficient (Q33) of 0.73 m4 C−2, far exceeding those of piezoceramics (0.034–0.096 m4 C−2). Piezoresponse force microscopy (PFM) analysis demonstrates the polarization switching and domain structure of 1 further confirming its ferroelectric nature. Furthermore, thermoplastic polyurethane (TPU) polymer composite films of 1 were prepared and employed as piezoelectric nanogenerators. Notably, the 15 wt % 1‐TPU device gave a maximum output voltage of 13.57 V and a power density of 6.03 μW cm−2. [ABSTRACT FROM AUTHOR]