Large Room-Temperature Magnetoresistance in a High-Spin Donor-Acceptor Conjugated Polymer.

Open-shell conjugated polymers (CPs) offer new opportunities for the development of emerging technologies that utilize the spin degree of freedom. Their light-element composition, weak spin-orbit coupling, synthetic modularity, high chemical stability, and solution-processability offer attributes that are unavailable from other semiconducting materials. However, developing an understanding of how electronic structure correlates with emerging transport phenomena remains central to their application.

Ultrasensitive Room Temperature Infrared Photodetection Using a Narrow Bandgap Conjugated Polymer.

Photodetectors operating across the short-, mid-, and long-wave infrared (SWIR-LWIR, λ = 1-14 µm) underpin modern science, technology, and society in profound ways. Narrow bandgap semiconductors that form the basis for these devices require complex manufacturing, high costs, cooling, and lack compatibility with silicon electronics, attributes that remain prohibitive for their widespread usage and the development of emerging technologies. Here, a photoconductive detector, fabricated using a solution-processed narrow bandgap conjugated polymer is demonstrated that enables charge carrier generation in the infrared and ultrasensitive SWIR-LWIR photodetection at room temperature.

Retinomorphic Motion Detector Fabricated with Organic Infrared Semiconductors.

Organic retinomorphic sensors offer the advantage of in-sensor processing to filter out redundant static backgrounds and are well suited for motion detection. To improve this promising structure, here, the key role of interfacial energetics in promoting charge accumulation to raise the inherent photoresponse of the light-sensitive capacitor is studied. Specifically, incorporating appropriate interfacial layers around the photoactive layer is crucial to extend the carrier lifetime, as confirmed by intensity-modulated photovoltage spectroscopy.

Structural pseudocapacitors with reinforced interfaces to increase multifunctional efficiency.

Structural supercapacitors hold promise to expand the energy capacity of a system by integrating load-bearing and energy-storage functions in a multifunctional structure, resulting in weight savings and safety improvements. Here, we develop strategies based on interfacial engineering to advance multifunctional efficiency. The structural electrodes were reinforced by coating carbon-fiber weaves with a uniquely stable conjugated redox polymer and reduced graphene oxide that raised pseudocapacitive capacitance and tensile strength.

Magnetic Ordering in a High-Spin Donor-Acceptor Conjugated Polymer.

The development of open-shell organic molecules that magnetically order at room temperature,which can be practically applied, remains a grand challenge in chemistry, physics, and materials science. Despite the exploration of vast chemical space, design paradigms for organic paramagnetic centers generally result in unpaired electron spins that are unstable or isotropic. Here, a high-spin conjugated polymer is demonstrated, which is composed of alternating cyclopentadithiophene and benzo[1,2-c;4,5-c']bis[1,2,5]thiadiazole heterocycles, in which macromolecular structure and topology coalesce to promote the spin center generation and intermolecular exchange coupling.

Heterojunction bilayers serving as a charge transporting interlayer reduce the dark current and enhance photomultiplication in organic shortwave infrared photodetectors.

Previous approaches to induce photomultiplication in organic diodes have increased the photosignal but lacked control over reducing background noise. This work presents a new interlayer design based on a heterojunction bilayer that concurrently enables photomultiplication and suppresses the dark current in organic shortwave infrared detectors to improve the overall detectivity. The heterojunction bilayer consists of a hole-transporting material copper thiocyanate and an electron-transporting material tin oxide, and this combination offers the ability to block charge injection in the dark.

Broadband infrared photodetection using a narrow bandgap conjugated polymer.

Photodetection spanning the short-, mid-, and long-wave infrared (SWIR-LWIR) underpins modern science and technology. Devices using state-of-the-art narrow bandgap semiconductors require complex manufacturing, high costs, and cooling requirements that remain prohibitive for many applications. We report high-performance infrared photodetection from a donor-acceptor conjugated polymer with broadband SWIR-LWIR operation.

Gold-Catalyzed C-H Functionalization Polycondensation for the Synthesis of Aromatic Polymers.

Homogeneous gold (Au) complexes have demonstrated tremendous utility in modern organic chemistry; however, their application for the synthesis of polymers remains rare. Herein, we demonstrate the first catalytic application of Au complexes toward the polycondensation of alkyne-containing comonomers and heteroarene nucleophiles. Polymerization occurs through successive intermolecular hydroarylation reactions to produce high molecular weight aromatic copolymers with 1,1-disubstituted alkene backbone linkages.

A sensor array for the discrimination of polycyclic aromatic hydrocarbons using conjugated polymers and the inner filter effect.

Natural and anthropogenic activities result in the production of polycyclic aromatic hydrocarbons (PAHs), persistent pollutants that negatively impact the environment and human health. Rapid and reliable methods for the detection and discrimination of these compounds remains a technological challenge owing to their relatively featureless properties, structural similarities, and existence as complex mixtures. Here, we demonstrate that the inner filter effect (IFE), in combination with conjugated polymer (CP) array-based sensing, offers a straightforward approach for the quantitative and qualitative profiling of PAHs.

Silica-Supported Organolanthanum Catalysts for C-O Bond Cleavage in Epoxides.

Single-site organolanthanum complexes supported on mesoporous silica nanoparticles, La{C(SiHMe)}@MSNs, catalyze the ring-opening hydroboration reaction of aliphatic and styrenic epoxides with pinacolborane (HBpin). The surface-bound complexes, synthesized by reaction of the homoleptic tris(alkyl)lanthanum La{C(SiHMe)} and SBA-type MSN treated at 700 °C (MSN), are mostly monopodal ≡SiO-La{C(SiHMe)} and contain an average of one bridging La↼H-Si per alkyl ligand. This structure was established through a combination of solid-state NMR (SSNMR) experiments, including -resolved SiH coupling and quantitative Si measurements, diffuse reflectance IR, and elemental analysis.

Solution-Processed Phototransistors Combining Organic Absorber and Charge Transporting Oxide for Visible to Infrared Light Detection.

This report demonstrates high-performance infrared phototransistors that use a broad-band absorbing organic bulk heterojunction (BHJ) layer responsive from the visible to the shortwave infrared, from 500 to 1400 nm. The device structure is based on a bilayer transistor channel that decouples charge photogeneration and transport, enabling independent optimization of each process. The organic BHJ layer is improved by incorporating camphor, a highly polarizable additive that increases carrier lifetime.

Zirconium-catalyzed desymmetrization of aminodialkenes and aminodialkynes through enantioselective hydroamination.

The catalytic addition of alkenes and amines (hydroamination) typically provides α- or β-amino stereocenters directly through C-N or C-H bond formation. Alternatively, desymmetrization reactions of symmetrical aminodialkenes or aminodialkynes provide access to stereogenic centers with the position controlled by the substrate's structure. In the present study of an enantioselective zirconium-catalyzed hydroamination, stereocenters resulting from C-N bond formation and desymmetrization of a prochiral quaternary center are independently controlled by the catalyst and reaction conditions.