Conjugated terpolymers emerge as promising candidates to develop wearable and stretchable electronics for the merits of mechanical stretchability and high charge mobility. Despite their potential, backbone structural diversity causes significant variability and limited predictability in their electrical stretchability, hindering their rational design. Here, we report a rational design on the backbone structure for high-performance stretchable terpolymers. We study a novel group of terpolymers, DPP-mSe-nTz, with varying ratios of two co-monomer units. The frontier molecular orbital exhibits higher delocalization length with the increased ratio of DPP-Se segments. Accordingly, terpolymers with extended frontier molecular orbital exhibit superior electrical performance under strain. The optimized terpolymer (DPP-75Se) exhibits high hole mobility of 0.29 cm2 V-1 s-1 and high retention of 28% under 100% strain. Combining observation on the morphology evolution and computational analysis of charge transport, we propose a comprehensive understanding of frontier molecular orbital delocalization in enhancing the electrical stretchability of terpolymers.

Vinylene-linked covalent organic frameworks (COFs) are considered as one of the most promising COF materials due to their full π-conjugation and excellent stability. However, the irreversibility of carbon-carbon double bond formation can lead to uncontrolled nucleation and growth, limiting crystal growth and structural regulation of vinylene-linked COFs. Here, we leverage reversible protonation reactions between carboxylic acids and N-heteroaromatic precursors to realize controlled synthesis of vinylene-linked COFs and investigate their crystallization process in depth. Carboxylic acid acts as a modulator to precisely regulate the acidity of the melt polymerization system, which can slow the polymerization and nucleation rates, providing opportunities to correct molecular misconnection and promote the formation of thermodynamically more stable crystal structures. The synthesized N-heteroaromatic vinylene-linked COFs exhibited unprecedented crystal domains, with a maximum size up to 0.33 μm. The 15 N-heteroaromatic vinylene-linked COFs with high crystalline quality and excellent photochemical properties were successfully synthesized via this strategy. When used as a catalyst for oxygen reduction reactions, the new 2,2',6,6'-tetramethyl-4,4'-bipyridine/4,4″-p-terphenyldicarboxaldehyde (TMBP-TPDA) exhibited excellent performance, achieving a H2O2 generation rate of 17.53 mmol g-1 h-1 in pure water, surpassing existing COF-based photocatalysts. This study is not only searching for an efficient formula but also exploring and understanding the inherent laws of the reaction, paving the way for precise regulation and practical application of vinylene-linked COFs.

Organic-inorganic hybrid perovskites (OIHPs) offer a promising alternative, combining strong spin-orbit coupling, high carrier mobility, and tunable optoelectronic properties. However, their potential for spintronic applications has been constrained by rapid spin relaxation, often attributed solely to the inorganic sublattice. Here, we demonstrate room-temperature spin transport in hybrid perovskites enabled by isotope engineering. Substituting hydrogen with deuterium in methylammonium lead iodide effectively suppresses hyperfine interactions (HFI), leading to a 2.6-fold increase in spin lifetime. As a result, CD₃ND₃PbI₃ exhibits a magnetocurrent (MC) ratio of 17.5% at room temperature, whereas conventional CH₃NH₃PbI₃ spin-valve devices show negligible MC response. A spin photovoltaic effect is also observed under ambient conditions, revealing a coupling between optical excitation and spin-polarized transport, and pointing toward new opportunities for light-addressable spintronic functionality. These findings not only revise the fundamental understanding of spin relaxation in hybrid materials, but also establish isotope engineering as a powerful strategy to access room-temperature spin functionality.

Graphene and other single-layer two-dimensional van der Waals (vdW) crystals have been of great research interest for the past two decades, demonstrating the possible interest for research on single-chain one-dimensional (1D) vdW materials. Furthermore, 1D vdW materials are predicted to have interesting physics and find applications in subnanometre electronic devices, as their sizes in both dimensions are close to physical limits. Here we prepared independent, single-chain 1D vdW crystals in which the single chains feature a definite chemical structure with a width of approximately 0.8 nm, a length reaching the micrometre scale and a single-chain ratio up to 90%. Atomically smooth vdW interfaces resulting from the inherent intrachain closed covalent bonding were observed, accompanied by good crystal quality and air stability. Low temperature electron transport measurements of the 1D vdW chains revealed typical single-electron tunnelling characteristics, demonstrating the possible applications of these materials in quantum technologies.

The binding affinity of aptamer, which plays a key role in aptamer-based liquid biopsy, is affected by the unstable aptamer conformation. Existing strategies enhancing the binding affinity are complex, time-consuming, not easily generalizable, and lack universality to different aptamers. Herein, we discovered an interfacial electric locking effect and developed a universal strategy to stabilize aptamer conformations at the semiconductor-liquid interface. A positive liquid gate voltage redistributes the ions, forming a positively charged environment with an increasing cation concentration at the interface. The positive environment and the ionic interaction between the cations and phosphate backbone locks the aptamer conformation, decreasing the dissociation constant down to 10-10 M with universality to different aptamers. The platform based on this strategy monitors a wide range of analytes in less than 5 min with a lowest limit of detection down to 10-20 M. With such ultrasensitive detection capability, the platform demonstrates a robust classification accuracy of 98.6% in 51 clinical samples of bladder cancer.

Fullerene-based electron transport layers (ETLs) are commonly used in tin-based perovskite solar cells for high power conversion efficiency, but they suffer from high cost, complex synthesis, low electron mobilities and limited interaction with the perovskite. To tackle these issues, we use non-fullerene ETLs, that is, fluorinated triple-acceptor polymers (P1, P2 and P3), which offer lower cost, simpler synthesis, higher electron mobility and greater structural flexibility. These polymers form continuous, conformal interfaces with tin perovskite layers, enabling stronger, more uniform interactions, especially over large areas. Notably, P3 achieves optimal energy-level alignment and efficient electron transfer, resulting in efficiencies of 16.06% (certified at 15.90%) for 0.04-cm2 and 14.67% (certified at 14.51%) 1-cm2 devices, outperforming fullerene-based cells. Both devices retain over 85% of their initial efficiency after 550 h under continuous 1-sun illumination owing to the hydrophobicity of P3's long-alkyl side chains and fluorine substituents. This study shows the potential of non-fullerene ETLs for tin perovskite photovoltaics.

ABSTRACT Covalent organic frameworks (COFs) featuring donor–acceptor architectures have shown great promise as photocatalysts. However, their performance is often hindered by limitations such as narrow absorbance ranges and restricted electron delocalization, which are inherent to traditional imine linkages. Herein, we introduce a fused‐ring acceptor–π–acceptor (FRA–π–A) architecture for near‐infrared‐absorbing COFs, enabled via in situ COF‐to‐COF transformation that replaces imine linkages with FRA‐derived benzodithiazoles (or benzodioxazoles). Comprehensive structural characterizations confirm their mesoporous crystalline structure, featuring pore size distribution of 2.16–2.39 nm and broad light absorption extending to near‐infrared region. Property investigations demonstrate that the rigid backbones derived from the FRA–π–A architecture significantly enhance long‐range in‐plane electron delocalization, thereby improving the separation and transport of photogenerated charge carriers. Crucially, the accelerated carrier migration preferentially directs photogenerated electrons to the FRAs, promoting the formation of •O 2 − radicals and accelerating the rate‐limiting step of the oxygen reduction reaction. These synergistic structural and optoelectronic properties endow the FRA–π–A COFs with an outstanding photocatalytic H 2 O 2 production rate of 6.8 mmol g − 1 h − 1 without sacrificial agents, exceeding the vast majority of conjugated linkage‐based COFs. This study highlights the immense potential of FRA–π–A COFs as high‐performance photocatalysts.

The rapid development of the Internet of Things and wearable technologies has created substantial demand for stretchable optoelectronic devices. Among these, intrinsically stretchable organic optoelectronic devices are emerging as key technologies for applications in wearable electronics, electronic skin, and health monitoring. This review systematically summarizes the recent progress in this field. We first outline two primary strategies for achieving stretchability: structural engineering (buckling and island-bridge configurations) and intrinsic material design. The review focuses on the latter, providing a comprehensive overview of the design of key components, including insulators, electrodes, and optoelectronic functional layers. Specifically, the design principles for intrinsically stretchable semiconductor active layers are elaborated with a focus on molecular engineering and composite material strategies. Furthermore, we summarize the performance optimization and applications of representative devices, such as organic photodiodes (OPDs), organic phototransistors (OPTs), organic photovoltaics (OPVs), organic light-emitting diodes (OLEDs), and organic light-emitting electrochemical cells (OLECs). The potential of these devices for integrated systems, including human-machine interaction, neuromorphic electronics, and wearable health monitors, is also explored. Finally, the current challenges and future research directions are discussed.

With the ongoing advancements in experimental techniques for two-dimensional conjugated polymers (2DCPs), significant reductions in disorder and the flourishing methods for structural manipulation have attracted increasing interest in their electronic structures. The tight-binding model taking molecular orbitals as the basis provides a conceptual framework for structural and functional design; however, further investigation is needed concerning the influence of secondary frontier orbitals and model construction in slipped-stacking multilayer structures. In this article, we concentrate on models for tetrahedral homopolymers, examining the role of secondary frontier orbitals through a recombined orbital basis. Results show that while a single-orbital model can give band structures that closely align with density functional theory calculations, including additional orbitals based on symmetry and phase considerations yields clearer chemical insights and facilitates straightforward extensions to multilayer systems. In particular, we emphasize a double-orbital model featuring a pair of linearly extended orbitals that cross at the center of the building block. Enhanced destructive quantum interference is observed in homopolymers compatible with this model when subjected to van der Waals interactions from an adjacent layer exhibiting a slipped stacking configuration. Through this crossed double-orbital model, the origins of the quantum interference can be effectively elucidated. Furthermore, we show that the doping-induced spin polarization in bilayers compatible with this model can be controlled by interlayer interference, a phenomenon for which our extended model provides an effective framework for analyzing.

Point-of-care (POC) testing holds great promise for transforming clinical diagnostics by enabling rapid, convenient, and accurate analysis outside of centralized laboratories. Among various emerging technologies, biological field-effect transistors (bio-FETs), which directly convert molecular binding events into electrical signals, are gaining attention as strong candidates for next-generation POC diagnostic platforms due to their label-free operation, fast response, and ease of integration. The core functionality of bio-FETs lies at the solution-solid interface, where molecular recognition and signal transduction occur simultaneously. The physicochemical characteristics of this interface determine whether low-abundance molecular binding events can be effectively distinguished from background noise. However, under real clinical conditions, this interface is often compromised by strong ionic shielding and nonspecific adsorption, leading to signal attenuation and instability, factors that significantly hinder the clinical translation of bio-FET technology. In this Account, we summarize our group's advances in biochemical interface engineering for bio-FETs, with a focus on improving molecular recognition and signal transduction to enhance device performance in POC diagnostic applications. For molecular recognition, interfaces were designed that enhance probe-target binding affinity while minimizing nonspecific interactions. Nuclease-mediated recognition mechanisms were introduced to achieve sequence-specific detection with single-nucleotide resolution. These strategies enable bio-FETs to capture molecular binding events more efficiently and convert them into reliable electrical signals. In terms of signal transduction, multiple approaches were employed to localize binding events within the Debye length, enrich analytes at the sensing surface, and stabilize weak or transient molecular interactions, effectively transforming them into quantifiable electrical outputs. These methods improve recognition sensitivity while reducing background noise and signal drift in complex biological media, resulting in clearer and more consistent readouts. Interface-engineered bio-FETs have successfully detected a wide range of clinically relevant biomarkers, including nucleic acids, proteins, metabolites, and reactive oxygen species, with limits of detection (LoDs) as low as 10-18 M, response times under 5 min, and operational stability in undiluted clinical samples. We have further developed portable POC diagnostic prototypes that integrate bio-FETs with the accompanying software, supporting parallel, multitarget detection and data analysis. These platforms have demonstrated rapid and accurate detection of SARS-CoV-2, Zika virus, Mycobacterium tuberculosis, hepatocellular carcinoma, prostate cancer, and diabetes in complex clinical matrices, highlighting their strong potential for practical deployment. Collectively, these advances underscore the pivotal role of biochemical interface engineering in translating bio-FETs from proof-of-concept studies into clinically relevant diagnostic platforms. Finally, we outline the opportunities and challenges associated with advancing bio-FETs as comprehensive biodetection platforms for future applications. We believe that continued progress in biochemical interface engineering will further enhance the practical capabilities of bio-FETs and provide essential technical support for developing a new generation of high-performance bioelectronic diagnostic systems.

Two pyrimidoisoindigo-based polymers were synthesized by copolymerizing thiophene-flanked pyrimidoisoindigo (T-PymII) with thiophene (T) or 3,4-difluorothiophene (2FT), and their structure-property correlations were investigated. Although both polymers exhibited ambipolar transport properties, P(PymII-TTT was dominated by hole transport, while P(PymII-T-2FT-T) was dominated by electron transport. Among them, the highest hole mobility up to 1.66×10−2 cm2·V−1·s−1 was observed for P(PymII-TTT), while the highest electron mobility of 6.37×10−3 cm2·V−1·s−1 was observed for P(PymII-T-2FT-T). AFM and GIWAXS analyses revealed that their poor morphology and crystallinity may account for their inferior performance. Therefore, further side-chain engineering is needed to improve the crystallinity of PymII-based polymers.

The optoelectronic synapse is essential for integrating visual perception and information processing but remains constrained by limited charge-carrier separation and lifetime in photosensitive materials. Here, we introduce a dimensionality modulation strategy to construct one-dimensional (1D) and two-dimensional (2D) carbazole-porphyrin (Cz-Por) donor-acceptor (D-A) covalent organic frameworks (COFs) by tailoring Cz connectivity. Systematic studies reveal that the 1D-Cz-Por-COF exhibits more efficient charge separation and prolonged carrier dynamics, as evidenced by lower exciton binding energy and longer exciton lifetime compared with its 2D analogue. Consequently, neuromorphic transistors based on 1D-Cz-Por-COF/graphene heterojunctions achieve high photoresponsivity of 2.08 × 105 A W−1 and enhanced synaptic functions, including excitatory postsynaptic current, paired-pulse facilitation (157%), and long-term plasticity. Device arrays further enable accurate pattern recognition and broadband multicolor sensing. This work highlights dimensionality as a key regulator of COF carrier behavior and provides a promising materials platform for neuromorphic vision technologies.

n-Type organic semiconductors are indispensable components of organic optoelectronic devices and are central to the advancement of flexible electronics, bioelectronics and integrated organic circuits. Despite substantial progress, the development of high-performance acceptor building blocks and their corresponding n-type polymers remains fundamentally challenged by the difficult balance among frontier molecular orbital energetics, charge-transport capability and synthetic accessibility. In this context, boron-nitrogen (BN) motifs, including three-coordinate B-N bonds and four-coordinate B ← N bonds, have emerged as versatile molecular design elements for engineering electron-deficient π-conjugated systems. Owing to their unique isoelectronic characteristics and intrinsic bond polarization, BN units can effectively lower lowest unoccupied molecular orbital energy levels, enhance electron deficiency, and modulate intermolecular interactions while preserving favourable backbone planarity. As a result, they offer broad opportunities for simultaneously tuning optical bandgaps, charge-transport properties and environmental stability. In this review, we provide a comprehensive overview of BN-embedded electron-deficient small molecules and conjugated polymers, with particular emphasis on molecular design principles, synthetic methodologies and emerging structure-property relationships. We further discuss representative applications of these materials in five major optoelectronic device platforms, highlighting how BN structural characteristics govern electronic structure, solid-state organization and device performance. Finally, we outline the key challenges that remain in this rapidly evolving field and present perspectives on the future development of BN-enabled n-type organic semiconductors. This review aims to offer a unified framework and practical guidance for the rational design of next-generation high-performance n-type organic electronic materials.

The increasing demand for flexible displays and wearable electronics has driven extensive efforts to develop stretchable organic light-emitting diodes (OLEDs). A critical challenge in this field is the creation of emissive layers that combine high efficiency with mechanical robustness. Thermally activated delayed fluorescence (TADF) materials have attracted significant attention as third-generation emitters capable of achieving 100

Most clustered regularly interspaced short palindromic repeats (CRISPR)-based electrochemical biosensors lack controllable switching function and are vulnerable to false signals induced by intrinsic amplification signal crosstalk. Thus, exploring strategies that mitigate intrinsic amplification crosstalk with a precise switch would be extremely useful for reliable and accurate bioanalysis. Herein, we develop a photo-switchable CRISPR/Cas12a electrochemical (PSCE) system by introducing a photocleavable (PC) linker and adopting a light-responsive strategy, which enables output of de-interference electrochemical signals and achieves highly sensitive and accurate detection of gene mutations for non-small cell lung cancer (NSCLC). The system decouples nucleic acid amplification (NAA) from signal transduction and produces unique photo-switchable response signals by light irradiation to activate Cas12a activity. This architectural design further separates signal readout from sample pretreatment, suppressing intrinsic amplification-derived signal crosstalk rather than global biological interference to deliver an ultralow limit of detection (LoD). The PSCE achieves 98.1% sensitivity, 92.7% specificity, and 98.9% overall accuracy when tested with 67 clinical samples. Moreover, the exploration of PSCE system in flexible wearable electronics and machine-learning analysis of clinical patient samples demonstrates significant application potential clinical diagnosis of mutation-associated diseases.

ABSTRACT Developing intrinsically stretchable and healable semiconducting polymers with high charge‐carrier mobility is critical for next‐generation flexible electronics; however, integrating these conflicting functionalities remains a formidable challenge. Here, we report a “quadruple‐hydrogen‐bonds end‐capping” strategy to realize high‐performance stretchable and healable semiconducting polymers. By incorporating quadruple hydrogen‐bonds between end‐capping units linked with alkyl spacers into polymer backbone, we engineer a supramolecular architecture that achieves enhanced crystallinity and improved ordered packing with reduced π‐π stacking distance, and also superior stretchabillity with molecular‐ordering retention during stretching. Moreover, enhanced chain mobility together with dynamic and reversible and hydrogen‐bonding sites in the architecture contribute to efficient healing. Consequently, our designed semiconducting polymer exhibits a more than 2‐fold increase in mobility, while demonstrating stable mobility retention under strain, high mobility recovery after healing, and scalability in fully stretchable transistor arrays. This work provides an effective molecular design strategy for achieving simultaneous improvements in electrical performance, mechanical stretchability, and healing ability in organic electronics.

The electron-transporting layer (ETL) plays a crucial role in tin-based perovskite solar cells (TPSCs). However, the high synthesis cost, low mobility, and poor photothermal stability of the widely adopted ETL indene-C60 bisadduct (ICBA) limit TPSC development. Herein, we design and synthesize two n-type semiconducting polymers-PNDI-BT and PNDI-FBT-using direct arylation polymerization as alternative ETLs. Notably, the synthesis cost of PNDI-FBT is only 6% that of ICBA, making it a highly economical option. Both PNDI-BT and PNDI-FBT exhibit better performance compared to ICBA, offering cascade energy-level alignment, enhanced electron mobility, and improved photothermal stability. The fluorinated polymer PNDI-FBT shows even higher electron mobility and stronger interfacial interactions. Thus, the inverted TPSCs incorporating PNDI-FBT as the ETL achieve a remarkable power conversion efficiency of 15.57%, which significantly surpasses that of devices using ICBA (13.34%) and the nonfluorinated counterpart PNDI-BT (14.22%). These findings underscore the potential of n-type polymers as cost-effective ETLs for efficient TPSCs.