Surpassing the strength of metallogels with a rigid, amorphous metal-rich material formulation
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The properties of conducting polymers are strongly influenced by structural changes induced by long-range order, which can be achieved by using block copolymers that self-assemble into crystalline structures. These blends result in unique mesophases distinct from the pure components with self-assembly behavior modulated by solution conditions and polymer architectures. High-throughput small-angle X-ray scattering data of aqueous Pluronic P123 (PEO 20 –PPO 70 –PEO 20 ) and conjugated polyelectrolyte poly[3-(potassium-4-butanoate) thiophene-2,5-diyl] (PPBT) blends at various concentrations and temperatures were automatically classified into phase maps by autophasemap, an unsupervised statistical analysis algorithm. The outlined phase boundaries revealed that adding PPBT to high P123 concentrations induced a transition from cubicly ordered spherical micelles to hexagonally packed cylindrical micelles. Shear alignment via rheological small-angle neutron scattering of the blends produced monolithic oriented cubic and hexagonal crystal gels. Furthermore, these insights into the self-assembly of conductive polymer blends will aid in the design of soft materials with tunable structural and electronic properties.
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In response to escalating environmental concerns, there is a pressing demand for materials capable of delivering both sustainability and robust mechanical properties, thereby substituting nonrenewable counterparts in various applications. This study presents a comprehensive investigation into the synthesis and characterization of biobased aliphatic thermoplastic polyurethanes (TPUs) that exhibit impressive mechanical properties, including tensile strength in the range of 48–41 MPa and flexural modulus up to 2.2 GPa. These biodegradable TPUs displayed high shore A and D hardness between 95 and 98 and 51–42, respectively, and thus can be categorized as “extra hard” plastics according to the durometer scale for PUs. Herein, we have prepared a series of four 100% biobased polyester polyols from biobased diacid and chain-extender as precursors with molecular weights varying from 500 to 1400 g/mol. The corresponding TPUs that were prepared by using an aliphatic diisocyanate were evaluated for their thermal stability, microphase separation, mechanical properties, and biodegradation. By leveraging renewable feedstocks, these TPUs offer a sustainable alternative to petroleum-derived materials, with their mechanical performance meeting conventional benchmarks. Furthermore, postcomposting analysis revealed significant surface degradation, affirming their biodegradability and environmental compatibility.
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Paramagnetic transition metal complexes can serve as quantum bits, storing phase information through unpaired electrons. Despite their promise, these systems often require low temperatures and tend to rapidly decohere. Recent efforts have sought to improve longitudinal relaxation (T 1 ), which provides an upper limit for phase coherence (T m ), by investigating existing literature compounds with reduced vibrational coupling and orbital angular momentum. However, synthetic strategies for improving T 1 through novel ligand design have remained scant. Here, we disclose the synthesis of a new modular macrocyclic ligand framework with four nitrogen donors (N 4 ) derived from phenanthroline that supports room-temperature coherent Cu(II) spin centers. The optimized complex more than doubles the T 1 over the next best Cu(II)-N 4 compound and exhibits a room temperature coherence time (T m ) of 0.28 μs, close to previously reported values. This performance enhancement arises from a tight binding site with short Cu–N distances, resulting in a stronger ligand field and reduced thermal accessibility of symmetric vibrational modes. This work demonstrates a practical approach to enabling spin coherence at room temperature, a factor critical to accessing relevant quantum bits and biological sensors, through a designer macrocyclic ligand platform.
The efficiency of two-dimensional Dion–Jacobson-type materials relies on the complex interplay between electronic and lattice dynamics; however, questions remain about the functional role of exciton–phonon interactions. Here we establish the robust polaronic nature of the excitons in these materials at room temperature by combining ultrafast spectroscopy and electronic structure calculations. We show that polaronic distortion is associated with low-frequency (30–60 cm –1 ) lead iodide octahedral lattice motions. More importantly, we discover how targeted ligand modification of this two-dimensional perovskite structure manipulates exciton–phonon coupling, exciton polaron population and carrier cooling. At high excitation density, stronger exciton–phonon coupling increases the hot-carrier lifetime, forming a hot-phonon bottleneck. Furthermore, our study provides detailed insight into the exciton–phonon coupling and its role in carrier cooling in two-dimensional perovskites relevant for developing emerging hybrid semiconductor materials with tailored properties.
We report a series of redox-active bis(pincer) Pd( ii ) complexes in which the redox active units are based on either a diarylamido or a carbazolide framework.
The inherent selectivity of anion receptors can be reversed by ion pairing occurring both inside and outside of the receptor cavity.
The electro-active third component (BID)-incorporated PM6-B10-based organic solar cell shows a high performance (PCE = 17.2%) and mechanical stretchability (COS avg = 11.4%), outperforming the PM6-based device (PCE = 15.8%, COS avg = 2.0%).
The multiexciton quintet state, 5 TT, generated as a singlet fission intermediate in pairs of molecular chromophores, is a promising candidate as a qubit or qudit in future quantum information science schemes.
Motivated by recent studies of two-phase lipid vesicles possessing 2D solid domains integrated within a fluid bilayer phase, we study the shape equilibria of closed vesicles possessing a single planar, circular inclusion.
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We demonstrate the possibility to tune the saturation magnetization, coercivity, and uniaxial in-plane anisotropy constant in amorphous bilayers and multilayers of Co 85 (Al 70 Zr 30 ) 15 and Sm 11 Co 82 Ti 7 through the interface density. From magnetometry and x-ray circular dichroism (XMCD) measurements, we conclude that the easy-axis coercivity μ 0 H c increases four times when the number of bilayer repetitions, N, increases from 1 to 10 within a constant total sample thickness of 20 nm. At the same time, the anisotropy constant K u also increases by a factor four, whereas the saturation magnetization M s decreases slightly. The Co spin and orbital moments, m s and m l , are found to be approximately constant within the sample series. The average total Co moment is only 0.8-0.9 μ B /atom, but the m l /m s ratio is strongly enhanced compared to pure Co. Magnetization curves extracted from XMCD measurements show that the Co and Sm moments are ferromagnetically coupled for all samples.