Aggregate (Hoboken, N.J.)最新文献

Cancer is the leading cause of death worldwide, accounting for nearly 10 million deaths in 2020. The early diagnosis of cancer biomarkers is essential for improving prognosis and reducing the global disease burden. However, conventional diagnostic methods depend on sophisticated instrumentation, well-trained personnel, and complex workflows, which is usually time-consuming and costly. With programmable and sequence-specific nucleic acid recognition and cleavage, clustered regularly interspaced short palindromic repeats (CRISPR)-Cas systems have emerged as powerful tools for disease diagnostics. Their integration with engineering approaches, such as microfluidic devices including paper-based microfluidics, electrochemical, and smartphone-enabled platforms, has further enhanced cost-effectiveness, portability, and automation. This review presents the molecular mechanisms of CRISPR-Cas systems, recent advances in point-of-care testing (POCT) and its compatible technologies, and their applications in early cancer detection. We also discuss key challenges and future directions to enable accessible and reliable CRISPR-enabled diagnostics for improved global cancer diagnostics and provide the potential solution for effective treatment.

Liquid crystal elastomers (LCEs) have emerged as attractive soft actuators capable of undergoing large and reversible actuation. Their potential for practical applications, however, has been fundamentally constrained by an intrinsic trade-off: the chain flexibility required for reversible actuation inherently restricts molecular design toward achieving high mechanical strength and toughness. Here, we report a phase separation strategy that yields an LCE with a tensile strength of 92 MPa and toughness of 247 MJ m⁻³. This leads to 20-fold and 40-fold improvements compared with conventional LCEs without sacrificing their reversible actuation. Mechanistically, this superior mechanical performance is enabled by the incorporation of rigid polyamide acid segments into the network. During network formation, these segments self-assemble into phase-separated nanostructures that function as in situ-generated nanofillers, reinforcing the material and endowing it with outstanding work capacity. Our work suggests that leveraging microphase separation substantially broadens the design space for high-performance LCE actuators, paving the way toward mechanically robust and efficient soft actuation systems.

We report a new chiral indaceno[1,2-b:5,6-b′]dithiophene bis-thiophenylpropynone (IDT-TPO) dye exhibiting very noticeable chiroptical properties in thin films. While freshly prepared samples are ECD-silent, aging triggers a giant dichroic response, with ellipticity values reaching approximately 18,000 mdeg, among the highest reported to date for thin films of chiral organic dyes as neat materials. This amplification is accompanied by an unusual flattening of the main UV-Vis absorption band, and the combination of these effects produces very large g_abs values (exceeding 0.1). A thorough investigation, combining microscopy and spatially resolved chiroptical techniques with time-dependent density functional theory (TD-DFT) calculations, reveals that the intense chiroptical activity arises primarily from the consistent formation of right-handed three-dimensional (3D) helical architectures. Notably, the degree of circular polarization exhibits a non-monotonic dependence on film thickness: the maximum ECD intensity was found for a thinner film, rather than for the thickest one. This behavior is particularly promising for optoelectronic applications requiring efficient chiroptical responses in relatively thin active layers.

Metal–polyphenol networks (MPNs), as supramolecular functional materials formed through coordination-driven self-assembly of polyphenol ligands and metal ions (Fe²⁺, Cu²⁺, etc.), have demonstrated broad application prospects in the biomedical field due to their structural designability, excellent biocompatibility, and stimulus-responsive degradation properties. MPNs allow for precise control over coordination kinetics, stability, and functionality through diverse combinations of polyphenols and metal ions. Various assembly methods, including the template method, nanoprecipitation, layer-by-layer self-assembly, and one-pot synthesis, have successfully led to the construction of diverse structures such as films, nanoparticles, hollow capsules, hydrogels, and metal–organic frameworks. By adjusting the metal-to-polyphenol ratio, pH, reaction time, and introducing functional molecules, the size, surface charge, mechanical properties, and dissociation behavior of MPNs can be effectively controlled to meet the demands of various biomedical applications. Leveraging the synergistic interaction between paramagnetic or fluorescent metal ions and polyphenol structures, MPNs are widely used in the design of probes for magnetic resonance imaging, fluorescence imaging, photoacoustic imaging, and multimodal imaging, enabling precise localization and real-time monitoring of pathological sites. MPNs not only serve as highly efficient drug delivery carriers, enabling targeted release in response to the micro acidic or high reactive oxygen species environments of tumors, but also play a critical role in synergistic disease therapy through the enzymatic-like catalytic activity, photothermal conversion capabilities, and radiosensitizing effects of metal ions. In this review, we summarize the advances of MPNs as a highly versatile and functionally integrated supramolecular assembly platform, and discuss their pivotal role in steering biomedical materials away from single-function designs and toward intelligent, unified diagnostic and therapeutic solutions.

Strong near-infrared-II (NIR-II, 1000–1700 nm) absorbers with high photothermal efficiency are highly desirable for deep-tissue photoacoustic imaging and photothermal therapy. However, donor–acceptor (D–A) molecular design strategies that simultaneously achieve structural robustness and intense NIR-II absorption remain scarce. Herein, we demonstrate that single-boron coordination can be implemented on the intrinsically strong acceptor [1,2,5]thiadiazolo[3,4-g]quinoxaline (TQ), an unachieved regime by previously reported boron-engineered strategies, which have typically been based on weaker electron-deficient acceptors. Single intramolecular N→B–N coordination converts TQ into an even stronger electron-deficient motif than the widely used benzobis(thiadiazole) (BBT) acceptor. Through donor engineering and planarity modulation, the resulting borylated TQ derivative, BLD3, exhibits intense NIR‑II absorption with a high molar extinction coefficient (ε > 3 × 10⁴ M⁻¹ cm⁻¹) around 1000 nm in toluene. Featuring an ultrafast nonradiative decay of 2.1 ps, BLD3 nanoparticles (NPs) show a high photothermal conversion efficiency of 68% under 1060 nm laser irradiation, as well as a robust photoacoustic (PA) output under 1064 nm excitation. Combining excellent photo/thermal stability, favorable tumor accumulation, and good biocompatibility, BLD3 NPs enable effective NIR-II PA imaging-guided photothermal therapy with pronounced tumor ablation. This work expands the library of strong acceptors for boron‑coordination chemistry, providing a general platform for constructing powerful electron‑deficient building blocks and high‑performance NIR‑II phototheranostic materials.

The aggregate form of interorganelle interaction is essential for the stable operation of cellular energy metabolism, signal transduction, as well as growth and development. Among these, the discovery of lipid droplet–mitochondria interactions (LDMIs) mediated by their aggregation has reshaped the understanding of how intracellular lipid metabolic networks operate within cells. Complex spatiotemporal interactions between lipid droplets and mitochondrial aggregates are commonly observed at the subcellular level, supporting the stable and efficient cycling of lipids and energy within the cell. Advanced techniques enabling organelle aggregation manipulation with high spatiotemporal precision have emerged as critical tools for investigating LDMIs and addressing diseases associated with LDMI dysregulation. This study aimed to summarize and update the distinctive characteristics of LDMIs and highlight the increasing understanding of their operational mechanisms, while also examining diseases caused by their dysfunction. Special emphasis was placed on the current challenges and prospects of strategies for the spatial aggregation manipulation of LDMIs, particularly the remarkable potential of optogenetic tools. With the continuous advancement of subcellular imaging and organelle aggregation manipulation technologies, LDMIs are poised to transform our understanding of cellular lipid metabolism networks and facilitate the effective manipulation of these complex networks at the organelle level.

Accurate tumor boundary delineation is critical for successful surgical resection, yet achieving high-contrast imaging of hepatocellular carcinoma (HCC) remains challenging due to nonspecific liver accumulation and high intrinsic fluorescence of optical agents. Herein, we reported a molecular design strategy exploiting enhanced cyanine H-aggregation by dimerization, which enabled glutathione (GSH) responsive high-contrast HCC imaging and precise surgical navigation. Four cyanine dimers with different side-chains were constructed via molecular engineering. Among them, the propyl-substituted dimer DCy-Pr exhibited exceptionally low intrinsic fluorescence quantum yield (Φ_f < 0.01%) due to strong H-aggregation-caused quenching, achieving the highest GSH-triggered fluorescence turn-on (151.0-fold). However, the other three cyanine dimers with hydrophilic side chains (polyethylene glycol, anionic SO₃⁻, or cationic ammonium) showed unsatisfactory properties, such as absence of H-aggregation, no reactivity with GSH, and high intrinsic fluorescence. DCy-Pr displayed a remarkable fluorescence quenching, which outperformed its monomeric counterpart Cy-Azo (16.0-fold higher background fluorescence). Moreover, in vivo studies revealed that DCy-Pr efficiently accumulated in tumor regions, achieving remarkable fluorescence contrast with 9.7-fold tumor-to-normal tissue and 5.1-fold tumor-to-liver fluorescence ratios. Finally, DCy-Pr enabled precise delineation of orthotopic hepatic tumor margins and facilitated successful identification and resection of peritoneal metastatic nodules. In summary, this work not only presented a molecular design paradigm through modulating cyanine H-aggregation but also advanced precision surgery of HCC by providing credible real-time tumor margins.

Perovskite solar cells (PSCs) are promising next-generation photovoltaics, yet their efficiency promotion from lab-scale prototypes to industrial application is fundamentally hindered by interfacial instability and non-radiative recombination. These critical bottlenecks stem from complex defect chemistry, ion migration, energetic mismatches and material degradation at the perovskite heterojunction interface, which conventional empirical strategies often fail to address systematically. This perspective evaluates two pivotal paradigms for multidimensional top interfacial regulation: multimolecular synergistic systems, which utilize cooperative interactions among diverse functional additives, and all-in-one molecular integration, which employs sophisticated, multifunctional single molecules. We analyze how these distinct philosophies influence defect passivation kinetics, energy level alignment, operational resilience against ionic migration and environmental stressors. While multimolecular systems offer modular versatility, all-in-one integration provides superior structural precision to suppress phase separation and interfacial delamination. Furthermore, we assess their comparison and applicable scenarios. Finally, we propose a transition from empirical trial-and-error to data-driven predictive design. By establishing a unified molecular engineering framework, this paper provides a strategic roadmap for bridging the gap between research breakthroughs and reliable, commercially viable perovskite modules.

Red emitters suitable for solid-state applications are the subject of intense research. However, their development is delicate because, in general, the more the emission is red-shifted, the more its efficiency decreases. In this work, two series of phosphorescent tricarbonylrhenium complexes were synthesized and studied, both theoretically and experimentally. Their organic ligand is a phenyl-substituted quinoline or quinoxaline derivative. They also differ in their ancillary ligand, chloride or triphenylphosphine (TPP), and the presence of a bulky adamantyl substituent, initially introduced to improve the solid-state arrangement and thus the light emission efficiency. Unsurprisingly, chlorido complexes were not luminescent in solution, and only quinoline derivatives emitted faint red light in the solid state. In contrast, phosphino complexes were weakly phosphorescent in solution and showed strong solid-state luminescence enhancement. A red emission was observed for the microcrystalline powders of quinoxaline derivatives, with a PLQY up to 43%, a performance rarely achieved in this spectral region. This effect was attributed to the double intra- and intermolecular stabilization provided by the TPP moiety. The phosphino complexes were very well suited to aggregation-induced phosphorescence emission (AIPE) experiments. Their potential interest for related applications was shown. An adamantyl-substituted complex was used for the detection of sodium deoxycholate by taking advantage of the competition between these two compounds for a $�\beta$-cyclodextrin. Until now, phosphino tricarbonylrhenium complexes have been mainly exploited for their photodecarbonylation properties useful in phototherapy. This work shows that they are photostable after proper chemical modifications, and that their unique spectroscopic properties make them the leaders of a new generation of red emitters.