Cell Reports Physical Science最新文献

Achieving control over the transport properties of charge carriers is a crucial aspect of realizing high-performance electronic materials. In metal-halide perovskites, which offer convenient manufacturing traits and tunability for certain optoelectronic applications, this is challenging: the perovskite structure itself poses fundamental limits to maximum dopant incorporation. Here, we demonstrate an organic modifier incorporation strategy capable of modulating the electronic density of states in halide tin perovskites without altering the perovskite lattice, in a similar fashion to substitutional doping in traditional semiconductors. By incorporating organic small molecules and conjugated polymers into cesium tin iodide (CsSnI₃) perovskites, we achieve carrier density tunability over 2.7 decades, transition from a temperature-dependent semiconducting to a metallic nature, and high electrical conductivity exceeding 200 S/cm. We leverage these tunable and enhanced electronic properties to achieve a thin-film, lead-free, thermoelectric material with a near room temperature figure of merit of 0.21.

Optogenetics promises to manipulate the brain circuitry by exciting or inhibiting the same neurons via different colors of light (i.e., bidirectionality), and furthermore, to co-work with electrophysiology for low-crosstalk, high-resolution probing of the brain. Limited by feasible integration methods, though, neural probes with close-packed dual-color light sources remain underdeveloped, making high-resolution bidirectional in vivo optogenetic electrophysiology technically challenging. Here, we report, based on heterogeneously stacked III–V epitaxial films, a monolithic neural probe integrated with close-packed dual-color micro-light-emitting diodes (LEDs) and microelectrodes in 20- and 50-μm pitches, respectively. The resulting devices enable bidirectional in vivo optogenetic electrophysiology across layers IV and V of mouse somatosensory cortex, where dual-color LEDs are observed to excite and inhibit layer-specific brain dynamics. Such interlayer bidirectional in vivo optogenetic studies, to which our scalable probes are well suited, can add to high-resolution interrogation of the brain circuitry and shed light on animal disease models.

A primary focus among researchers is to reduce the energy required for CO₂ capture. Here, we report a system designed to capture CO₂ while simultaneously generating electricity. The reaction heat of amine-CO₂ in the point-source CO₂-capture process is harvested. Amine-functionalized mixtures (TEPA-SBA/MEA+PZ) exhibit 52% higher reaction enthalpy compared to primary amine absorbents. A membrane composed of tetraethylenepentamine-impregnated poly(ethylene glycol) dimethacrylate is employed, which selectively permeates CO₂ and minimizes heat loss by separating the flue gas channel and solvent reservoir. CO₂ working capacity of TEPA-SBA/MEA+PZ is 6.6 mmol/g under steady-state conditions of 15 mol % CO₂/N₂. Electricity can be harvested at a rate of 7.5 kJ/kg, and direct utilization of thermal energy yields 445 kJ/kg (net thermal energy consumption is 2.2 MJ/kg). While the proposed system has the potential to reduce CO₂ emissions from power plants to 0.25 ton/MWh and increase total electricity production by 0.6%, addressing device energy penalties remains a significant challenge.

The development of efficient processes for the preparation of structurally diverse axially chiral biaryls has been an important goal in synthetic organic chemistry and asymmetric catalysis. However, in sharp contrast to the well-established open-chain biaryls, the catalytic enantioselective construction of medium-sized bridged biaryls remains underdeveloped. In particular, no enantioselective synthesis of such frameworks possessing a configurationally stable stereogenic C-N axis with step- or pot-economy has been disclosed. Herein, we report a practical synthesis of atropisomeric eight-membered lactam-bridged N-arylindoles through a conceptually intriguing stepwise cut-and-sew strategy. The key to success lies in the development of a silver-catalyzed atroposelective ring-opening/cyclization cascade reaction of N-arylindole lactams with isocyanoacetates to establish C-N axial chirality. This method features operational simplicity, good functional group tolerance, high efficiency, as well as good to high enantiocontrol. It is also noteworthy that these scaffolds exhibit large Stokes shifts, demonstrating their potential applications as fluorescent dyes.

Three-dimensional (3D) interconnects increase chip power density and enable miniaturization. Photonic chips require new processes to enable transitioning to 3D interconnects. We fabricate 3D interconnects on a multijunction solar cell, leveraging processes such as III-V heterostructure plasma etching, gold electrodeposition, and chemical-mechanical polishing to integrate through substrate vias to the heterostructure. Wafer bonding is used to handle 20-μm-thin III-V films. The strategy enables us to demonstrate photonic power devices having areas 3 orders of magnitude smaller compared to standard chips. The design also yields a small shading factor below 3%. Compared to miniaturized photonic power devices with two-dimensional connections, 3D interconnects achieve a 6-fold increase in wafer area use. These improvements will enhance the power yield per wafer while unlocking high-density and miniaturized devices for applications such as power over fiber, the internet of things, and microconcentrator photovoltaics.

Ceria is important for catalysis due to its ability to form and utilize oxygen vacancies during redox reactions. Understanding the dynamic formation of the oxygen vacancies has contributed to the development of efficient catalytic processes. Here, we demonstrate the presence of oxygen vacancy clusters in the bulk of ceria and gold/ceria catalysts upon anaerobic carbon monoxide oxidation and describe their interplay with the orbital hybridization of Ce³⁺ 4f and 5d states. Observations are made using in situ X-ray Raman scattering spectroscopy at O K- and Ce N_4,5-edges and in situ X-ray diffraction. These, combined with multiplet calculations, allow detection of the formation of Ce³⁺ in gold/ceria upon low temperature carbon monoxide oxidation. The modifications observed at the O K-edge reflect the rearrangement of the bulk oxygen sublattice. Density-functional theory calculations show vacancy ordering in the bulk, and explain modifications at the O K-edge, involving the hybridization of the Ce 4f and 5d and O 2p orbitals.

Soft actuators offer several advantages over traditional rigid machines. Among soft materials, liquid metal (LM) is particularly noteworthy for its electro-responsive surface properties that induce flow or morphological changes, making it ideal for soft machines. Although using LM droplets as micropumps is simple, they face challenges in efficient vertical fluid pumping. Here, we report a pump-valve dual-functional LM soft actuator (PDLMA) that can continuously pump liquid upward. Benefiting from the unique conformability of LM, the PDLMA can provide the function of a check valve, which blocks the backflow of the rising liquid while continuing the pumping effect. At 6 V direct current (DC), the PDLMA lifts the solution more than 80 cm. We demonstrate the device’s applications in circuit-on/off switches and pump-mixer systems. Moreover, as a conceptual experiment, we show the PDLMA’s ability to achieve contamination-free drug delivery. The PDLMA represents a crucial step toward the development of soft actuators for flexible machines.

Deuterium labeling of organic molecules with high efficiency is a promising and challenging task in organic synthesis and drug discovery. Here we report two practical and robust strategies based on zinc-mediated one-pot reductive coupling of alkyl halides and (deuterated) alcohols utilizing ArSO₂SNa as crucial sulfur shuttle in absence of thiols. The approaches feature nickel and base-free conditions, broad substrate scope, and late-stage molecule modification, providing a wide range of trideuteromethyl alkyl sulfides and other important analogs with the examples of sulfoxide, sulfone, and sulfoximine. Initial mechanistic studies show that an active adduct of Zn into thiosulfonates is formed in nearly quantitative yield, and it could be further applied to the nucleophilic substitution of alkyl electrophiles to construct a variety of Csp³–S bonds.

Carbon-fiber-reinforced polymers (CFRPs) offer improved energy efficiency in aerospace and automobile applications due to lightweight and mechanical robustness but face challenges with limited recyclability and frequent fiber-polymer delamination caused by inadequate interfacial adhesion. Here, we report an effective design of tough and closed-loop recyclable carbon-fiber-reinforced vitrimers (CFRVs) with exceptional interfacial adhesion through the synergy of a boronic ester-modified commodity polymer, multidiol cross-linker, and diol-functionalized carbon fibers (CFs). The dynamic covalent bonding between the vitrimer and fiber interface results in 43% higher interfacial adhesion than that of CFRVs with pristine CFs. Moreover, CFRVs with diol-CFs exhibit ∼731-MPa tensile strength, 26% higher than unmodified CFRVs and 49% higher than conventional epoxy CFRPs. Importantly, the dynamic boronic ester exchange enables CFRV closed-loop recyclability, repairability, fast thermoformability, self-adhesion, and multicycle processability without compromising mechanical performance. The designed dynamic fiber-matrix interaction will open up a new paradigm of multifunctional CFRPs while providing a path toward closed-loop structural materials.

Small-molecule fluorophores in the second near-infrared window (NIR-II, 1,000–1,700 nm) have received widespread attention owing to their great breakthrough in deep-tissue imaging with high spatial resolution, but the strategies used to construct NIR-II fluorescent scaffolds are still very limited. Here, we report a pathway toward NIR-II wavelength-emissive fluorescent dyes, namely diphenylaminoacridine (DPA) dyes, with large Stokes shifts based on the planarized intramolecular charge transfer mechanism. DPAs exhibit tunable optical properties with the maximal absorption/emission wavelengths at 900 nm and 1,085 nm. They show high tolerance toward both photobleaching and oxidation. The in vivo gastrointestinal tract with high resolution demonstrates their significant potential in bioimaging. Overall, this work provides a promising avenue to construct NIR-II small-molecule fluorescent scaffolds for bioimaging.