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  1. Free, publicly-accessible full text available March 15, 2025
  2. Abstract

    Breath ammonia is an essential biomarker for patients with many chronic illnesses, such as chronic kidney disease (CKD), chronic liver disease (CLD), urea cycle disorders (UCD), and hepatic encephalopathy. However, existing breath ammonia sensors fail to compensate for the impact of breath humidity and complex breathing motions associated with a human breath sample. Here, a multimodal breath sensing system is presented that integrates an ammonia sensor based on a thermally cleaved conjugated polymer, a humidity sensor based on reduced graphene oxide (rGO), and a breath dynamics sensor based on a 3D folded strain‐responsive mesostructure. The miniaturized construction and module‐based configuration offer flexible integration with a broad range of masks. Experimental results present the capabilities of the system in continuously detecting diagnostic ranges of breath ammonia under real, humid breath conditions with sufficient sensing accuracy and selectivity over 3 weeks. A machine‐learning algorithm based on K‐means clustering decodes multimodal signals collected from the breath sensor to differentiate between healthy and diseased breath concentrations of ammonia. The on‐body test highlights the operational simplicity and practicality of the system for noninvasively tracing ammonia biomarkers.

     
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    Free, publicly-accessible full text available February 10, 2025
  3. Low-dimensional organic/inorganic hybrid perovskites (OIHPs) are a promising class of materials with a wide range of potential applications in optoelectronics and other fields since these materials can synergistically combine individual features of organic molecules and inorganics into unique properties. Non-covalent interactions are commonly observed in OIHPs, in particular, π-effect interactions between the organic cations. Such non-covalent interactions can significantly influence important properties of the low-dimensional OIHPs, including dielectric confinement, bandgap, photoluminescence, quantum efficiency, charge mobility, trap density, stability, and chirality. This perspective reviews recent studies of non-covalent interactions involving the π systems of organic cations in low-dimensional OIHPs. The analysis of crystal structures of low-dimensional OIHPs offers significant insight into understanding such non-covalent interactions and their impacts on specific properties of these OIHPs. The developed structure–property relationships can be used to engineer non-covalent interactions in low-dimensional OIHPs for applications. 
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    Free, publicly-accessible full text available June 12, 2024
  4. Demonstrated is the successful A 2 + B 2 RAFT step-growth polymerization of bis-acrylamides using a bifunctional trithiocarbonate chain transfer agent as the comonomer. Remarkably, homopropagation typical of acrylamides leading to branching and crosslinking was not observed. Moreover, synthesized poly(acrylamides) can be degraded by simply adding excess ethanolamine or PBu 3 . 
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    Free, publicly-accessible full text available May 30, 2024
  5. Abstract

    Flexible electronics have received considerable attention in the past decades due to their promising application in rollable display screens, wearable devices, implantable devices, and other electronic applications. In particular, conjugated polymers are favored for flexible electronics due to their mechanical flexibility and potential for solution‐processed fabrication techniques, such as blade‐coating, roll‐to‐roll printing, and high‐throughput printing allowing for high‐performance transistor devices. Thiophene is the prevailing conjugated unit to construct these conjugated polymers due to its favorable electronic properties. On the other hand, furans are among the few conjugated moieties that are easily derived from bio renewable resources. To promote sustainability, we selectively introduced furan into the conjugated backbone of a high‐mobility polymer scaffold and systematically studied the effect on the microstructure and charge transport. We show that partially and selectively replacing thiophene units with furan can yield nearly comparable performance compared to the all‐thiophene polymer. This strategy offers an improvement in the sustainability of the polymer by incorporating bio‐sourced furan without sacrificing the high‐performance characteristics. Meanwhile, polymers with incorrect or complete furan incorporation show reduced mobilities. This work serves to develop coherent structure–morphology–performance relationships; such knowledge will establish guidelines for the future development of sustainable, furan‐based conjugated materials.

     
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  6. Photomediated RAFT step-growth polymerization was performed with and without the presence of a photocatalyst using a trithiocarbonate-based CTA and a maleimide monomer. Under catalyst-free conditions, the polymerization proceeded with an appreciable rate under irradiation with blue and green light, which was extended to red light in the presence of ZnTPP. 
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  7. Conventional time-of-flight (TOF) measurements yield charge carrier mobilities in photovoltaic cells with time resolution limited by the RC time constant of the device, which is on the order of 0.1–1 µs for the systems targeted in the present work. We have recently developed an alternate TOF method, termed nonlinear photocurrent spectroscopy (NLPC), in which carrier drift velocities are determined with picosecond time resolution by applying a pair of laser pulses to a device with an experimentally controlled delay time. In this technique, carriers photoexcited by the first laser pulse are “probed” by way of recombination processes involving carriers associated with the second laser pulse. Here, we report NLPC measurements conducted with a simplified experimental apparatus in which synchronized 40 ps diode lasers enable delay times up to 100 µs at 5 kHz repetition rates. Carrier mobilities of ∼0.025 cm2/V/s are determined for MAPbI3 photovoltaic cells with active layer thicknesses of 240 and 460 nm using this instrument. Our experiments and model calculations suggest that the nonlinear response of the photocurrent weakens as the carrier densities photoexcited by the first laser pulse trap and broaden while traversing the active layer of a device. Based on this aspect of the signal generation mechanism, experiments conducted with co-propagating and counter-propagating laser beam geometries are leveraged to determine a 60 nm length scale of drift velocity dispersion in MAPbI3 films. Contributions from localized states induced by thermal fluctuations are consistent with drift velocity dispersion on this length scale.

     
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