ACS Earth and Space Chemistry最新文献

Immunofluorescence assays are extensively used for the detection of disease-associated biomarkers within patient samples for direct diagnosis. Unfortunately, these 2D microarrays suffer from low repeatability and fail to attain the low limits of detection (LODs) required to accurately discern disease progression for clinical monitoring. While three-dimensional microarrays with increased biorecognition molecule density stand to circumvent these limitations, their viscous component materials are not compatible with current microarray fabrication protocols. Herein, we introduce a platform for 3D microarray bioprinting, wherein a two-step printing approach enables the high-throughput fabrication of immunosorbent hydrogels. The hydrogels are composed entirely of cross-linked proteins decorated with clinically relevant capture antibodies. Compared to two-dimensional microarrays, these proteinaceous microarrays offer 3-fold increases in signal intensity. When tested with clinically relevant biomarkers, ultrasensitive single-plex and multiplex detection of interleukin-6 (LOD 0.3 pg/mL) and tumor necrosis factor receptor 1 (LOD 1 pg/mL) is observed. When challenged with clinical samples, these hydrogel microarrays consistently discern elevated levels of interleukin-6 in blood plasma derived from patients with systemic blood infections. Given their easy-to-implement, high-throughput fabrication, and ultrasensitive detection, these three-dimensional microarrays will enable better clinical monitoring of disease progression, yielding improved patient outcomes.

Enabling reversible control over the topological invariants, transitioning them from nontrivial to trivial states, has fundamental implications for quantum information processing and spintronics. It offers a promising avenue for establishing an efficient on/off switch mechanism for robust and dissipationless spin-currents. While mechanical strain has traditionally been advantageous for such manipulation of topological invariants, it often comes with the drawback of in-plane fractures, rendering it unsuitable for high-speed, time-dependent operations. This study employs ultrafast optical and THz spectroscopy to explore topological phase transitions induced by light-driven strain in Bi₂Se₃. Bi₂Se₃ requires substantial strain for Z₂ switching. Our observations provide experimental evidence of ultrafast switching behavior, demonstrating a transition from a topological insulator with spin-momentum-locked surfaces to hybridized states and normal insulating phases under ambient conditions. Notably, applying light-induced strong out-of-plane strain effectively suppresses surface-bulk coupling, facilitating the differentiation of surface and bulk conductance even at room temperature─significantly surpassing the Debye temperature. We expect various time-dependent sequences of transient hybridization and manipulation of topological invariant through photoexcitation intensity adjustments. The sudden surface and bulk transport alterations near the transition point enable coherent conductance modulation at hypersound frequencies. Our findings on the potential of light-triggered ultrafast switching of topological invariants hold promise for high-speed topological switching and its related applications.

Efficient electrochemical Li⁺ adsorption holds significant promise for lithium extraction, while the mismatched rate between Li⁺ diffusion and electron transport within the electrode material impedes the electrochemical activity and restricts the adsorption efficiency. To address this challenge, herein, we rationally design and integrate the ion and electron dual-conducting poly(vinyl alcohol)-polyaniline (PVA-PANI) copolymer (CP) within the H_1.6Mn_1.6O₄ (HMO) electrode matrix to facilitate Li⁺ diffusion and electron transport. The Li⁺ diffusion coefficient (D_Li+) increased from 3.03 × 10^-10 to 5.92 × 10^-10 cm²/s, while the charge transfer resistance (R_ct) decreased from 53.73 to 29.57 ohm. Consequently, the HMO@CP electrode exhibits superior adsorption kinetics and a state-of-the-art high adsorption capacity of up to 49.48 mg/g. Comprehensive mechanistic studies reveal that the negatively charged hydroxyl groups (-OH) in PVA accelerate Li⁺ diffusion and that the conjugated structure and redox-active quinoid sites in PANI offer denser electron distribution and promote electron transport. This synergistic effect in CP significantly enhanced Li⁺ diffusion and electron transport, leading to electrochemical activity and adsorption efficiency. Our work highlights the critical role of simultaneously regulating the ion diffusion and electron transport dual pathways for optimizing Li⁺ adsorption performance and inspires development of the next generation electrochemical adsorption electrodes.

Dark exciton states show great potential in condensed matter physics and optoelectronics because of their long lifetime and rich distribution in band structures. Therefore, they can theoretically serve as efficient energy reservoirs, providing a platform for future applications. However, their optical-transition-forbidden nature severely limits their experimental exploration and hinders their current application. Here, we demonstrate a universal dark state nonlinear energy transfer (ET) mechanism in monolayer WS₂/CsPbBr₃ van der Waals heterostructures under two-photon excitation, which successfully utilizes the enormous energy reserved in the dark exciton state of CsPbBr₃ to significantly improve the photoelectric performance of monolayer WS₂. We first propose the scenario of resonant ET between the dark state of CsPbBr₃ and WS₂, and then reveal that this is a typical Förster resonant ET and belongs to the 2D-2D category. Interestingly, the dark state ET in CsPbBr₃ is identified as a long-range donor-bridge-acceptor hopping mode, with a potential distance exceeding 200 nm. Finally, we successfully achieve nearly an order of magnitude enhancement in the near-infrared detection performance of monolayer WS₂. Our results enrich the theory of dark exciton states and ET, and they provide a way of using dark exciton states for future practical applications.