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.Improved understanding of passivation leads to near-infrared perovskite light-emitting diodes with 21.6% external quantum efficiency.
A universal method to obtain record‐high electronic Seebeck coefficients is demonstrated while preserving reasonable conductivities in doped blends of organic semiconductors through rational design ...of the density of states (DOSs). A polymer semiconductor with a shallow highest occupied molecular orbital (HOMO) level‐poly(3‐hexylthiophene) (P3HT) is mixed with materials with a deeper HOMO (PTB7, TQ1) to form binary blends of the type P3HTx:B1‐x (0 ≤ x ≤ 1) that is p‐type doped by F4TCNQ. For B = PTB7, a Seebeck coefficient S = 1100 µV K−1 with conductivity σ = 0.3 S m−1 at x = 0.10 is achieved, while for B = TQ1, S = 2000 µV K−1 and σ = 0.03 S m−1 at x = 0.05 is found. Kinetic Monte Carlo simulations with parameters based on experiments show good agreement with the experimental results, confirming the intended mechanism. The simulations are used to derive a design rule for parameter tuning. These results can become relevant for low‐power, low‐cost applications like (providing power to) autonomous sensors, in which a high Seebeck coefficient translates directly to a proportionally reduced number of legs in the thermogenerator, and hence in reduced fabrication cost and complexity.
Record‐high Seebeck coefficients are achieved for p‐type‐doped blends of common conjugated polymers. The method used is based on a rational design of the density of states, such that the characteristic hop occurs from the compound with the shallower HOMO to the compound with the deeper HOMO.
Conducting polymers, such as the p-doped poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), have enabled the development of an array of opto- and bio-electronics devices. However, ...to make these technologies truly pervasive, stable and easily processable, n-doped conducting polymers are also needed. Despite major efforts, no n-type equivalents to the benchmark PEDOT:PSS exist to date. Here, we report on the development of poly(benzimidazobenzophenanthroline):poly(ethyleneimine) (BBL:PEI) as an ethanol-based n-type conductive ink. BBL:PEI thin films yield an n-type electrical conductivity reaching 8 S cm
, along with excellent thermal, ambient, and solvent stability. This printable n-type mixed ion-electron conductor has several technological implications for realizing high-performance organic electronic devices, as demonstrated for organic thermoelectric generators with record high power output and n-type organic electrochemical transistors with a unique depletion mode of operation. BBL:PEI inks hold promise for the development of next-generation bioelectronics and wearable devices, in particular targeting novel functionality, efficiency, and power performance.
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.
Nonfullerene (NF) organic solar cells (OSCs) have been attracting significant attention in the past several years. It is still challenging to achieve high‐performance flexible NF OSCs. NF acceptors ...are chemically reactive and tend to react with the low‐temperature‐processed low‐work‐function (low‐WF) interfacial layers, such as polyethylenimine ethoxylated (PEIE), which leads to the “S” shape in the current‐density characteristics of the cells. In this work, the chemical interaction between the NF active layer and the polymer interfacial layer of PEIE is deactivated by increasing its protonation. The PEIE processed from aqueous solution shows more protonated N+ than that processed from isopropyl alcohol solution, observed from X‐ray photoelectron spectroscopy. NF solar cells (active layer: PCE‐10:IEICO‐4F) with the protonated PEIE interfacial layer show an efficiency of 13.2%, which is higher than the reference cells with a ZnO interlayer (12.6%). More importantly, the protonated PEIE interfacial layer processed from aqueous solution does not require a further thermal annealing treatment (only processing at room temperature). The room‐temperature processing and effective WF reduction enable the demonstration of high‐performance (12.5%) flexible NF OSCs.
Protonation of polyethylenimine ethoxylated (PEIE) can effectively passivate the chemical reaction between the PEIE and a nonfullerene (NF) active layer. As a result, the PEIE can work very efficiently as a low‐work‐function interface for NF solar cells. These flexible solar cells exhibit power conversion efficiency up to 12.5% with a room‐temperature‐processed PEIE interface.
Developing environmentally friendly perovskites has become important in solving the toxicity issue of lead‐based perovskite solar cells. Here, the first double perovskite (Cs2AgBiBr6) solar cells ...using the planar structure are demonstrated. The prepared Cs2AgBiBr6 films are composed of high‐crystal‐quality grains with diameters equal to the film thickness, thus minimizing the grain boundary length and the carrier recombination. These high‐quality double perovskite films show long electron–hole diffusion lengths greater than 100 nm, enabling the fabrication of planar structure double perovskite solar cells. The resulting solar cells based on planar TiO2 exhibit an average power conversion efficiency over 1%. This work represents an important step forward toward the realization of environmentally friendly solar cells and also has important implications for the applications of double perovskites in other optoelectronic devices.
Cs2AgBiBr6 films composed of high‐crystal‐quality grains with diameters equal to the film thickness are fabricated. These high‐quality double‐perovskite films show electron–hole diffusion lengths greater than 100 nm, enabling the fabrication of planar‐structure double‐perovskite solar cells with a maximum value of 1.22%.
Doping of organic semiconductors is crucial for the operation of organic (opto)electronic and electrochemical devices. Typically, this is achieved by adding heterogeneous dopant molecules to the ...polymer bulk, often resulting in poor stability and performance due to dopant sublimation or aggregation. In small-molecule donor-acceptor systems, charge transfer can yield high and stable electrical conductivities, an approach not yet explored in all-conjugated polymer systems. Here, we report ground-state electron transfer in all-polymer donor-acceptor heterojunctions. Combining low-ionization-energy polymers with high-electron-affinity counterparts yields conducting interfaces with resistivity values five to six orders of magnitude lower than the separate single-layer polymers. The large decrease in resistivity originates from two parallel quasi-two-dimensional electron and hole distributions reaching a concentration of ∼10
cm
. Furthermore, we transfer the concept to three-dimensional bulk heterojunctions, displaying exceptional thermal stability due to the absence of molecular dopants. Our findings hold promise for electro-active composites of potential use in, for example, thermoelectrics and wearable electronics.
Molecular doping is a crucial tool for controlling the charge-carrier concentration in organic semiconductors. Each dopant molecule is commonly thought to give rise to only one polaron, leading to a ...maximum of one donor:acceptor charge-transfer complex and hence an ionization efficiency of 100%. However, this theoretical limit is rarely achieved because of incomplete charge transfer and the presence of unreacted dopant. Here, we establish that common p-dopants can in fact accept two electrons per molecule from conjugated polymers with a low ionization energy. Each dopant molecule participates in two charge-transfer events, leading to the formation of dopant dianions and an ionization efficiency of up to 200%. Furthermore, we show that the resulting integer charge-transfer complex can dissociate with an efficiency of up to 170%. The concept of double doping introduced here may allow the dopant fraction required to optimize charge conduction to be halved.
Record power conversion efficiencies (PCEs) of perovskite solar cells (PSCs) have been obtained with the organic hole transporter 2,2′,7,7′-tetrakis(
N
,
N
-di-
p
...-methoxyphenyl-amine)9,9′-spirobifluorene (spiro-OMeTAD). Conventional doping of spiro-OMeTAD with hygroscopic lithium salts and volatile 4-
tert
-butylpyridine is a time-consuming process and also leads to poor device stability. We developed a new doping strategy for spiro-OMeTAD that avoids post-oxidation by using stable organic radicals as the dopant and ionic salts as the doping modulator (referred to as ion-modulated radical doping). We achieved PCEs of >25% and much-improved device stability under harsh conditions. The radicals provide hole polarons that instantly increase the conductivity and work function (WF), and ionic salts further modulate the WF by affecting the energetics of the hole polarons. This organic semiconductor doping strategy, which decouples conductivity and WF tunability, could inspire further optimization in other optoelectronic devices.
A radical doping approach
In perovskite solar cells, high power conversion efficiencies (PCEs) are usually obtained with an organic hole transporter called spiro-OMeTAD. This material must be doped to have sufficient conductivity and optimal work function, but the conventional process with lithium organic salts requires a long oxidation step that also affects device stability. Zhang
et al
. added spiro-OMeTAD biradical precursors that convert into stable organic monoradicals. Combined with ionic salts, this doping strategy formed solar cells with high PCEs (>25%) and improved stability. This approach also allows conductivity and work function to be tuned separately and could be applied in other optoelectronic devices. —PDS
Organic radicals and ionic salts enable doping of an organic hole transporter without post-oxidation treatments.
Prosthetic joint infection (PJI) is a prevalent and severe complication characterized by high diagnostic challenges. Currently, a unified diagnostic standard incorporating both computed tomography ...(CT) images and numerical text data for PJI remains unestablished, owing to the substantial noise in CT images and the disparity in data volume between CT images and text data. This study introduces a diagnostic method, HGT, based on deep learning and multimodal techniques. It effectively merges features from CT scan images and patients' numerical text data via a Unidirectional Selective Attention (USA) mechanism and a graph convolutional network (GCN)-based Feature Fusion network. We evaluated the proposed method on a custom-built multimodal PJI dataset, assessing its performance through ablation experiments and interpretability evaluations. Our method achieved an accuracy (ACC) of 91.4% and an area under the curve (AUC) of 95.9%, outperforming recent multimodal approaches by 2.9% in ACC and 2.2% in AUC, with a parameter count of only 68 M. Notably, the interpretability results highlighted our model's strong focus and localization capabilities at lesion sites. This proposed method could provide clinicians with additional diagnostic tools to enhance accuracy and efficiency in clinical practice.
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