Macroscopic Monograin Nano-Gyroid Thin Films in 4-inch Scale Through Shear-Rolling and Subsequent Solvent Annealing.

The gyroid structure from self-assembly is highly attractive for optical applications such as photonic crystals and metamaterials. However, due to the direction-dependent nature of these applications, achieving a monograin-level structure over a large area has remained challenging. In this study, the fabrication of unidirectionally oriented anisotropic nanocylinders of polystyrene-block-polydimethylsiloxane (PS-b-PDMS) is reported block copolymer thin films up to a 4-inch scale via a shear-rolling process, followed by solvent annealing to induce phase transition to nearly monograin gyroid structures.

Enhancing P2/O3 Biphasic Cathode Performance for Sodium-Ion Batteries: A Metaheuristic Approach to Multi-Element Doping Design.

Sodium-ion batteries (SIBs) have emerged as a compelling alternative to lithium-ion batteries (LIBs), exhibiting comparable electrochemical performance while capitalizing on the abundant availability of sodium resources. In SIBs, P2/O3 biphasic cathodes, despite their high energy, require furthur improvements in stability to meet current energy demands. This study introduces a systematic methodology that leverages the meta-heuristically assisted NSGA-II algorithm to optimize multi-element doping in electrode materials, aiming to transcend conventional trial-and-error methods and enhance cathode capacity by the synergistic integration of P2 and O3 phases.

Suppression of Thermally Induced Surface Traps in Colloidal Quantum Dot Solids via Ultrafast Pulsed Light.

Thermal annealing (TA) of colloidal quantum dot (CQD) films is considered an important process for recent high-performing CQD solar cells (SCs) due to its beneficial effects on CQD solids, including enhanced electrical conductivity, denser packing of CQD films, and the removal of organic residues and solvents. However, the conventional TA for CQDs, which requires several  minutes, leads to hydroxylation and oxidation on the CQD surface, resulting in the formation of trap states and a subsequent decline in SC performance. To address these challenges, this study introduces a flashlight annealing (FLA) technique that significantly reduces the annealing time to the millisecond scale.

The Influence of Regiochemistry on the Performance of Organic Mixed Ionic and Electronic Conductors.

Thiophenes functionalised in the 3-position are ubiquitous building blocks for the design and synthesis of organic semiconductors. Their non-centrosymmetric nature has long been used as a powerful synthetic design tool exemplified by the vastly different properties of regiorandom and regioregular poly(3-hexylthiophene) owing to the repulsive head-to-head interactions between neighbouring side chains in the regiorandom polymer. The renewed interest in highly electron-rich 3-alkoxythiophene based polymers for bioelectronic applications opens up new considerations around the regiochemistry of these systems as both the head-to-tail and head-to-head couplings adopt near-planar conformations due to attractive intramolecular S-O interactions.

Hole Mobility Enhancement in Benzo[1,2-b:4,5-b']Dithiophene-Based Conjugated Polymer Transistors through Directional Alignment, Perovskite Functionalization and Solid-State Electrolyte Gating.

Tunability in electronic and optical properties has been intensively explored for developing conjugated polymers and their applications in organic and perovskite-based electronics. Particularly, the charge carrier mobility of conjugated polymer semiconductors has been deemed to be a vital figure-of-merit for achieving high-performance organic field-effect transistors (OFETs). In this study, the systematic hole carrier mobility improvement of benzo[1,2-b:4,5-b']dithiophene-based conjugated polymer in perovskite-functionalized organic transistors is demonstrated.

Revealing Two Distinct Formation Pathways of 2D Wurtzite-CdSe Nanocrystals Using In Situ X-Ray Scattering.

Understanding the mechanism underlying the formation of quantum-sized semiconductor nanocrystals is crucial for controlling their synthesis for a wide array of applications. However, most studies of 2D CdSe nanocrystals have relied predominantly on ex situ analyses, obscuring key intermediate stages and raising fundamental questions regarding their lateral shapes. Herein, the formation pathways of two distinct quantum-sized 2D wurtzite-CdSe nanocrystals - nanoribbons and nanosheets - by employing a comprehensive approach, combining in situ small-angle X-ray scattering techniques with various ex situ characterization methods is studied.

Development of n-Type Small-Molecule Acceptors for Low Dark Current Density and Fast Response Organic Photodetectors.

Suppressing the dark current density () while maintaining sufficient charge transport is important for improving the specific detectivity (*) and dynamic characteristics of organic photodetectors (OPDs). In this study, we synthesized three novel small-molecule acceptors (SMAs) densely surrounded by insulating alkyl side chains to minimize the in OPDs. Introducing trialkylated N-annulated perylene diimide as a terminal moiety to the alkylated π-conjugated core structure was highly efficient in suppressing in the devices, resulting in an extremely low of 4.

Peculiar transient behaviors of organic electrochemical transistors governed by ion injection directionality.

Despite the growing interest in dynamic behaviors at the frequency domain, there exist very few studies on molecular orientation-dependent transient responses of organic mixed ionic-electronic conductors. In this research, we investigated the effect of ion injection directionality on transient electrochemical transistor behaviors by developing a model mixed conductor system. Two polymers with similar electrical, ionic, and electrochemical characteristics but distinct backbone planarities and molecular orientations were successfully synthesized by varying the co-monomer unit (2,2'-bithiophene or phenylene) in conjunction with a novel 1,4-dithienylphenylene-based monomer.

High-Performance Organic Electrochemical Transistors Achieved by Optimizing Structural and Energetic Ordering of Diketopyrrolopyrrole-Based Polymers.

For optimizing steady-state performance in organic electrochemical transistors (OECTs), both molecular design and structural alignment approaches must work in tandem to minimize energetic and microstructural disorders in polymeric mixed ionic-electronic conductor films. Herein, a series of poly(diketopyrrolopyrrole)s bearing various lengths of aliphatic-glycol hybrid side chains (PDPP-mEG; m = 2-5) is developed to achieve high-performance p-type OECTs. PDPP-4EG polymer with the optimized length of side chains exhibits excellent crystallinity owing to enhanced lamellar and backbone interactions.

Dissecting the Interplay between Organic Charge-Modulated Field-Effect Transistors and Field-Effect Transistors through Interface Control Engineering.

Organic charge-modulated field-effect transistors (OCMFETs) have garnered significant interest as sensing platforms for diverse applications that include biomaterials and chemical sensors owing to their distinct operational principles. This study aims to improve the understanding of driving mechanisms in OCMFETs and optimize their device performance by investigating the correlation between organic field-effect transistors (OFETs) and OCMFETs. By introducing self-assembled monolayers (SAMs) with different functional groups on the AlO gate dielectric surface, we explored the impact of the surface characteristics on the electrical behavior of both devices.

Effect of Fluorination Position on the Crystalline Structure and Stretchability of Intrinsically Stretchable Polymer Semiconductors.

A clear understanding of the structure-property relationship of intrinsically stretchable polymer semiconductors (ISPSs) is essential for developing high-performance polymer-based electronics. Herein, we investigate the effect of the fluorination position on the crystalline structure, charge-carrier mobility, and stretchability of polymer semiconductors based on a benzodithiophene--benzotriazole configuration. Although four different polymer semiconductors showed similar field-effect mobilities for holes (μ ≈ 0.

High Detectivity Near Infrared Organic Photodetectors Using an Asymmetric Non-Fullerene Acceptor for Optimal Nanomorphology and Suppressed Dark Current.

Recently, the development of non-fullerene acceptors (NFAs) for near-infrared (NIR) organic photodetectors (OPDs) has attracted great interest due to their excellent NIR light absorption properties. Herein, we developed NFAs by substituting an electron-donating moiety (branched alkoxy thiophene (BAT)) asymmetrically (YOR1) and symmetrically (YOR2) for the Y6 framework. YOR1 exhibited nanoscale phase separation in a film blended with PTB7-Th.

Thermal Management Enables Stable Perovskite Nanocrystal Light-Emitting Diodes with Novel Hole Transport Material.

The severely insufficient operational lifetime of perovskite light-emitting diodes (LEDs) is incompatible with the rapidly increasing external quantum efficiency, even as it approaches the theoretical limit, thereby significantly impeding the commercialization of perovskite LEDs. In addition, Joule heating induces ion migration and surface defects, degrades the photoluminescence quantum yield and other optoelectronic properties of perovskite films, and induces the crystallization of charge transport layers with low glass transition temperatures, resulting in LED degradation under continuous operation. Here, a novel thermally crosslinked hole transport material, poly(FCA -co-BFCA -co-VFCA ) (poly-FBV), with temperature-dependent hole mobility is designed, which is advantageous for balancing the charge injection of the LEDs and limiting the generation of Joule heating.

Manipulation and Direct Characterization of Polymer/Small-Molecule Interface Morphology in Bulk-Heterojunction Solar Cell.

To investigate the effect of miscibility between conjugated polymers (CPs) and Y6 on bulk-heterojunction (BHJ) type morphology, we propose three different CPs with similar chemical structures but different miscibility with Y6. After selectively removing Y6 from the CP/Y6 blend films, their interface morphology and interlocked dimensions are quantitatively compared using a square-wave model. As CP-Y6 miscibility increases, a higher intermixed interface is formed, providing an enlarged CP-Y6 interface area.

A Semi-Crystalline Polymer Semiconductor with Thin Film Stretchability Exceeding 200.

Despite the emerging scientific interest in polymer-based stretchable electronics, the trade-off between the crystallinity and stretchability of intrinsically stretchable polymer semiconductors-charge-carrier mobility increases as crystallinity increases while stretchability decreases-hinders the development of high-performance stretchable electronics. Herein, a highly stretchable polymer semiconductor is reported that shows concurrently improved thin film crystallinity and stretchability upon thermal annealing. The polymer thin films annealed at temperatures higher than their crystallization temperatures exhibit substantially improved thin film stretchability (> 200%) and hole mobility (≥ 0.

The Influence of Regiochemistry on the Performance of Organic Mixed Ionic and Electronic Conductors.

Thiophenes functionalised in the 3-position are ubiquitous building blocks for the design and synthesis of organic semiconductors. Their non-centrosymmetric nature has long been used as a powerful synthetic design tool exemplified by the vastly different properties of regiorandom and regioregular poly(3-hexylthiophene) owing to the repulsive head-to-head interactions between neighbouring side chains in the regiorandom polymer. The renewed interest in highly electron-rich 3-alkoxythiophene based polymers for bioelectronic applications opens up new considerations around the regiochemistry of these systems as both the head-to-tail and head-to-head couplings adopt near-planar conformations due to attractive intramolecular S-O interactions.

Impact of peripheral alkyl chain length on mesocrystal assemblies of G2 dendrons.

Unique sphere-packing mesophases such as Frank-Kasper (FK) phases have emerged from the viable design of intermolecular interactions in supramolecular assemblies. Herein, a series of C-G2-CONH dendrons possessing an identical core wedge are investigated to elucidate the impact of peripheral alkyl chain lengths (C) on the formation of the close-packed structures. The C and C dendrons, of which the contour lengths of the periphery are longer than the wedge length , assemble into a uniform sphere-packing phase such as body-centred cubic (BCC), whereas the C dendron with short ( < ) corona environment forms the FK A15 phase.

Helical polymers for dissymmetric circularly polarized light imaging.

Control of the spin angular momentum (SAM) carried in a photon provides a technologically attractive element for next-generation quantum networks and spintronics. However, the weak optical activity and inhomogeneity of thin films from chiral molecular crystals result in high noise and uncertainty in SAM detection. Brittleness of thin molecular crystals represents a further problem for device integration and practical realization of chiroptical quantum devices.

Repairable Macroscopic Monodomain Arrays from Block Copolymers Enabled by Photoplastic and Photodielectric Effects.

Upon exposure to UV light (120 mW/cm, λ = 365 nm), a - isomerization occurs in a cylinder-forming, azobenzene-containing block copolymer of polydimethylsiloxane--poly((4(phenyldiazenyl)phenoxy)hexyl acrylate) (PDMS--PPHA) that enables the generation of monodomains of healable, long-range ordered arrays of nanoscopic domains over macroscopic distances. The - isomerization gives rise to a significant increase in the dielectric constant (from 6.52 to 19.

Multiscale Convolutional Transformer for EEG Classification of Mental Imagery in Different Modalities.

A new kind of sequence-to-sequence model called a transformer has been applied to electroencephalogram (EEG) systems. However, the majority of EEG-based transformer models have applied attention mechanisms to the temporal domain, while the connectivity between brain regions and the relationship between different frequencies have been neglected. In addition, many related studies on imagery-based brain-computer interface (BCI) have been limited to classifying EEG signals within one type of imagery.

Kinetic-Controlled Crystallization of α-FAPbI Inducing Preferred Crystallographic Orientation Enhances Photovoltaic Performance.

Crystallization kinetic controls the crystallographic orientation, inducing anisotropic properties of the materials. As a result, preferential orientation with advanced optoelectronic properties can enhance the photovoltaic devices' performance. Although incorporation of additives is one of the most studied methods to stabilize the photoactive α-phase of formamidinium lead tri-iodide (α-FAPbI ), no studies focus on how the additives affect the crystallization kinetics.

Ionic Liquids for Intrinsically Stretchable Conductive Polymers.

Inspired by the classic hard-soft acid-base theory and intrigued by a theoretical prediction of spontaneous ion exchange between poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) and hard-cation-soft-anion ionic liquid (IL), we treat PEDOT:PSS with a new IL composed of a (., extremely hard) cation (3-methylimidazolium, -MIM) and an extremely soft anion (tetracyanoborate, TCB). In fact, this IL (-MIM:TCB) accomplishes the same levels of ion-exchange-mediated PEDOT-PSS separation, PEDOT-rich nanofibril formation, and electrical conductivity enhancement (∼2500 S/cm) as its counterpart (EMIM:TCB with 1-ethyl-3-methylimidazolium), the best IL used for this purpose so far.

Apex hydrogen bonds in dendron assemblies modulate close-packed mesocrystal structures.

The close-packed mesocrystal structures from soft-matter assemblies have recently received attention due to their structural similarity to atomic crystals, displaying various sphere-packing Frank-Kasper (FK) and quasicrystal structures. Herein, diverse mesocrystal structures are explored in second-generation dendrons (G2-X) designed with identical wedges, in which the terminal functionalities X = CONH and CHNH represent two levels of the strong and weak hydrogen-bonding apexes, respectively. The cohesive interactions at the core apex, referred to as the core interactions, are effectively modulated by forming heterogeneous hydrogen bonds between these two functional units.