Light-controlled peptide self-assembly provides a versatile platform for creating functional materials with high spatiotemporal precision. This review summarizes the physicochemical principles that enable optical control over self-assembly processes across thermodynamic and nonequilibrium regimes. Under thermodynamic control, light reshapes free-energy landscapes by modulating intermolecular interactions through photochemical reactions and photoisomerizations. To achieve nonequilibrium control, light can serve as a kinetic selector, directing assembly pathways to produce kinetically trapped states. It can also function as an energy driver, maintaining dissipative assemblies. Light-mediated systems chemistry strategies (e.g., reaction-diffusion, reaction networks, out-of-equilibrium conditions) further generate life-like properties, such as macroscopic patterning, metabolic self-replication, and adaptive evolution. Translational opportunities are highlighted in emerging biomedical applications, including precision cancer therapeutics, engineered cell culture, and programmable microbial regulation. Finally, key challenges and future directions are outlined in the development of light-coordinated intelligent peptide materials.
Cilia and their nucleating bodies, centrioles, are enigmatic structures in cell biology. The immotile primary cilium, lacking the motor proteins required to drive fluid flow, was widely considered vestigial throughout the 20th century; in sharp contrast, the modern understanding is that primary cilia are central to sensation, cellular differentiation, and metazoan development. This revolution has been guided by advances in molecular biology, high-resolution imaging, and the strict conservation of the cilia-centriole apparatus from the last eukaryotic common ancestor, empowering studies of model organisms across distant evolutionary lineages. Contemporaneously, the role of quantum mechanics in biology has progressed from trivial applications in bioorganic chemistry to the suspicion that life can tunnel, entangle, and establish extended quantum coherences within diverse families of proteins and nucleic acids. In explorations of eukaryotic quantum biology, many of the current protein systems of interest are found within the highly regulated microenvironment of the cilium, a geometrically precise aggregate. Consequently, we argue that understanding the cilium-centriole complex will require bridging classical biology with emerging quantum biophysics. In this review, we introduce the essential elements of quantum biology alongside the emerging frontiers of ciliary biology, aiming to facilitate interactions between these fields with an eye toward developing testable hypotheses of how nature may take advantage of quantum mechanics in this unique cellular environment.
Almost all high-performance acceptors currently rely on a single electron-withdrawing core or a core modified with electron-withdrawing groups, which significantly limits structural innovation. In this study, we introduced two novel extended electron-deficient units, [1, 2, 5]thiadiazolo[3,4-b]pyrazine (Tz-Qx) and [1, 2, 5]oxadiazolo[3,4-b]pyrazine (Dz-Qx), into the acceptor central cores. Coupled with fluorine and chlorine-substituted terminal groups, the performance of the acceptors can be synergistically optimized. A systematic investigation elucidates the impact of the central core and terminal groups on the intrinsic photoelectronic properties of the acceptors. Among the four acceptors—Tz-Qx-4F, Tz-Qx-4Cl, Dz-Qx-4F, and Dz-Qx-4Cl—Tz-Qx-4F demonstrated significant near-infrared absorption, excellent crystallinity, and enhanced aggregation capabilities. When blended with the polymer donor D18, the binary device achieved a remarkable power conversion efficiency (PCE) of 19.50%, accompanied by a record short-circuit current density (JSC) of 29.3 mA cm−2. This performance is attributed to the balanced charge transport properties and reduced non-radiative energy losses in the blend films. In stark contrast, Dz-Qx-based counterparts yielded substantially lower PCEs (∼9%), underscoring the profound influence of core heteroatom identity. This work highlights the critical influence of extended electron-deficient units and terminal groups on the molecular photovoltaic properties, providing valuable insights for the design of enhanced-performance organic solar cell acceptors.
The stealth properties of nanoparticles (NPs) constitute key parameters controlling colloidal stability and nonspecific interactions, which are critical for biological applications. To address the limitations of polyethylene glycol (PEG), commonly used for this purpose, we investigate polysarcosine (PSar) peptoid to determine the shortest chain length required to confer stealth properties to NPs. Polymeric NPs encapsulating rhodamine dye with a bulky hydrophobic counterion and bearing azide groups at their surface are functionalized by click chemistry with PSar of different lengths, ranging from 5 to 19 sarcosine units. The obtained peptoid-functionalized NPs show remarkable colloidal stability in physiological media, in contrast to bare polymeric NPs. An increase in the length of grafted PSar results in a reduction of the negative surface charge to near-neutral values and diminishes protein adsorption and aggregation in blood serum, as evidenced by fluorescence correlation spectroscopy. NPs grafted with 19-mer PSar show minimal nonspecific interactions with live cells and glass surfaces in a complex biological media, in contrast to their shorter PSar analogues and bare polymeric NPs. The developed stealth NPs bearing 19-mer PSar and HaloTag ligand enable specific targeting and imaging of proteins at the cell surface with minimized nonspecific interactions. The obtained results suggest that a relatively short PSar peptoid can be used for achieving stealth properties in polymeric NPs, allowing fabrication of the next-generation nanomaterials for bioimaging and biosensing applications. We foresee that the use of optimized short-chain PSar as a stealth shell could be extended to other types of functional nanomaterials, which can improve their safety, surface chemistry, and performance.
The self-electroluminescent (self-ECL) behaviors of tetraphenylethylene carboxyl derivatives (TPED-(COOH)x) during the anodic process are first reported in this work. This study establishes a genuine co-reactant-free self-ECL system driven by electrogenerated radical disproportionation, which is mechanistically distinct from classic annihilation and co-reactant-mediated ECL pathways. The self-ECL mechanism involves the disproportionation of electrogenerated TPED•+-(COO−)x radicals to directly populate a charge-transfer excited state, which then decays radiatively. The results of the structure-activity analysis indicate that the electronic structure (determined by the conjugation length and substitution position) and intermolecular packing interactions are more important than either the aggregation-induced emission property or the oxidation potential for self-ECL. Furthermore, numerous controlled experiments have confirmed that the carboxyl group is essential for triggering self-ECL and this strategy can be extended to other AIE molecules. Notably, 4″,4″″′,4″″″″,4″″″″″′-(ethene-1,1,2,2-tetrayl) tetrakis ([1,1′:4′,1″-terphenyl]-4-carboxylic acid) (H4TCTPE) achieved a high self-ECL efficiency of up to 411% (relative to Ru(bpy)32+, ΦECL = 5%). Under optimal experimental conditions, an immunosensor for superoxide dismutase 2 (SOD2) was constructed based on H4TCTPE, with a linear range of 0.01-100 ng/mL, a detection limit of 7.9 pg/mL, excellent selectivity, reproducibility, and stability, and was successfully applied to serum analysis. This work provides a theoretical basis and design principles for the development of next-generation self-ECL luminophores.
Portable phase-change composite (PCC) materials with rapid heat storage and leakage suppression capabilities are crucial for heating supply and temperature regulation under complex environmental conditions; however, their development remains challenging. Inspired by the serial multi-chamber water-retention architecture of Sphagnum, a polyimide/MXene/etched zeolitic imidazolate framework-8 phase-change energy storage composite platform (sPMZ) was designed. The biomimetic hierarchical porous architecture, featuring aligned microcavities and nanopores, generated multiscale capillary forces that effectively suppress phase-change material leakage, enabling a paraffin loading of 85.3% while maintaining structural integrity over repeated thermal charging-discharging cycles. The incorporation of the biomimetic architecture increased the specific surface area of the sPMZ platform by 1198%, enhanced the thermal conductivity of the resulting PCC prepared by paraffin impregnation into sPMZ by 43.7%, and delivered a melting enthalpy of 119.5 J·g−1 with a relative enthalpy efficiency of 94.6%. In addition, the photothermal conversion efficiency attained 90.7%. Through photothermal conversion measurements, practical irradiation assessments, and integrated control of energy storage and heat dissipation, the feasibility and tunability of the Sphagnum-inspired strategy were validated, paving the way for developing portable thermal storage devices with rapid heat charging and suppressed leakage.
The use of stimuli-responsive hydrogels in optoelectronics holds promise due to their capacity to turn chemical or physical stimuli into optical signals by virtue of network dynamics, swelling equilibria, and microstructure. This review provides an insight into the chemistry and microarchitecture of hydrogels that influence optical transduction via refractive index modulation, scattering, birefringence, diffraction, and transparency. The review also highlights the important classes of stimuli involved in adaptive optics, including light, temperature, magnetic fields, ionic environment, metabolites, and enzymes. The hierarchical structuring, nanocomposites, and photonic structures can be used to modulate the magnitude of these responses. An important finding is that the limitations in designing stimuli-responsive devices are not necessarily linked to the sensitivity of the material but rather with the challenge of combining optical quality, mechanical strength, reversibility, and stability in real-world environments. Another important challenge is the absence of standardized criteria for measuring optical modulation, kinetic response, fatigue, and biostability. Future research will rely on data-driven strategies, such as polymer informatics and machine learning.
Two-dimensional van der Waals magnetic semiconductors offer unprecedented opportunities to explore coupled magnetic and excitonic phenomena. Through femtosecond transient absorption spectroscopy and density functional theory calculations, we identify the charge-transfer band edge in CrSBr near 500 nm (2.48 eV) and correlate distinct photoluminescence (PL) channels with Cr3+ coordination environments. Temperature-dependent measurements reveal that 720 nm emission (PL1) persists across all temperatures, consistent with isolated Cr3+ centers; ∼920 nm emission (PL2) intensifies near the ferromagnetic (FM) transition (140 K); and 990 nm emission (PL3) appears only in thick samples below the antiferromagnetic (AFM) transition (132 K). Under strong perpendicular magnetic fields with 488 nm excitation, we observe a dark-state exciton at ∼850 nm, with anticorrelated intensity variations between PL1/dark-state and PL2/PL3, demonstrating field-tuned energy redistribution. These findings establish magnetic polaronic excitons in van der Waals semiconductors and enable manipulation of excitonic properties through magnetic order control.
Manual crystallization experiments have always been challenging, requiring extensive process development expertise and often resulting in unpredictable results. The crystallization process plays a critical role in the development of high-quality organic materials, which are essential for various industries such as pharmaceuticals, materials science, and electronics. Therefore, crystallization experiments are in urgent need of innovative methods to ensure consistency, efficiency, and scalability. Recent studies have shown that machine learning can effectively assist crystal detection and segmentation, thus providing a new way to optimize organic crystallization processes, improving both the speed and precision of crystal formation. However, a comprehensive review of machine learning-based approaches for organic crystallization process monitoring remains elusive. It is therefore necessary to review the machine learning technologies involved, their current applications, technical challenges, and development blueprints. In this work, we focus on the application scenarios, basic principles, and common tools of machine learning methods based on image detection and segmentation in effectively monitoring the crystallization process of organic crystals, especially the research on artificial intelligence technology in the detection of crystal size and morphology, monitoring, and optimization of crystallization processes. Through this work, we aim to provide the oretical references and practical guidance for researchers in related fields.
Generally, the required dominant J-aggregation and ordered molecular stacking via morphology optimization gives rise to red-shifted absorption spectrum with lower optical energy bandgap (Eg), resulting in the adverse effect on the open-circuit voltage (Voc) improvement in organic solar cells (OSCs). To maximize power-conversion efficiency (PCE), it is desirable to reduce the energy loss (Eloss) of OSCs to refrain from decreasing the Voc via rational morphology optimization. Herein, we reveal the effect of solid additive treatment on collaboratively optimizing the charge carrier dynamics and Eloss to maximize short-circuit current density and fill factor without decreasing the Voc of OSCs. In addition to improving the J-aggregation and molecular stacking of D18:N3 blend for efficient charge separation and transport, it is found that the biphenyl (BPh) additive treatment significantly reduces the Eloss to offset the lower Eg for maintaining the high Voc of OSCs. As a result, the BPh additive treatment shows remarkable effect in boosting the PCE of OSCs. In particular, the BPh additive treatment for the D18:N3:L8-BO-4Cl-based device significantly elevates the PCE from 18.95% to 20.10%.
Discrete 2:2 host-guest complexes provide a well-defined platform for correlating supramolecular structure with emergent photophysical behavior. Although γ-cyclodextrin (γ-CD) is widely used in aqueous host-guest chemistry, structurally well-defined 2:2 complexes and their formation mechanisms remain poorly understood. Here we report a γ-CD-mediated 2:2 host-guest complex formed with 1,3,6,8-tetrakis(4-carboxyphenyl)pyrene tetrasodium salt (TCP) and systematically elucidate its structural, mechanistic, and photophysical characteristics. Combined 1H NMR, 2D NMR, and DOSY analyses resolve the 2:2 architecture, while thermodynamic and kinetic studies reveal a multistep complexation network involving 1:1, 1:2, and 2:2 species, with dimerization providing the dominant thermodynamic driving force. The resulting 2:2 complex exhibits enhanced fluorescence emission and pronounced chiroptical responses, including circular dichroism and circularly polarized luminescence, arising from supramolecular chirality induced by the chiral γ-CD cavities. Importantly, analogous γ-CD-mediated 2:2 complexation and associated photophysical features are also observed for a tetraphenylethylene-based guest, indicating that this binding mode is not limited to a single chromophoric scaffold. This study clarifies how 2:2 host-guest complexes can form in γ-CD systems and provides mechanistic insight into the emergence of chiral photophysical properties in such complexes.
The escalating crisis of antimicrobial resistance poses an urgent threat to global public health. Conventional photodynamic therapy (PDT) is limited by oxygen dependence and restricted light penetration, which can compromise its therapeutic efficacy in the hypoxic microenvironment of deep abscesses. Herein, we report a positional isomer engineering strategy that transforms a thioxanthene (THX) scaffold into aggregation-induced emission luminogens (AIEgens) with fluorescence extending into the second near-infrared (NIR-II) window and dual-modal therapeutic capability. Theoretical and photophysical studies revealed that the para-configured isomer (Ph-p-THX) exhibited a smaller energy gap and higher oscillator strength than its meta-counterpart (Ph-m-THX). These electronic features provide more favorable singlet-triplet energy alignment, thereby supporting triplet-involved Type-I-dominant mixed reactive oxygen species (ROS) generation under hypoxic-relevant conditions associated with abscess microenvironments. In parallel, the narrowed energy gap and enhanced light-harvesting capability contribute to efficient photothermal conversion. As a result, Ph-p-THX enabled NIR-II imaging-guided treatment and exhibited superior antibacterial activity against methicillin-resistant Staphylococcus aureus (MRSA) abscesses in vivo. Overall, this study highlights positional isomerization as an effective strategy for optimizing THX-based AIE photosensitizers for antimicrobial theranostic applications.
The pursuit of high-performance color filters (CFs) for next-generation displays demands organic dyes with a wide color gamut, high color purity, low emissivity, and excellent processability. Herein, we report a rational molecular design strategy by integrating the nonalternant, polar azulene unit into the BODIPY scaffold to create three novel derivatives—AzBdpy-B, AzBdpy-G, and AzBdpy-R—tailored for blue, green, and red subpixel applications. By strategically varying the linkage sites (azulene 1-/2-positons to BODIPY α/β positions), we precisely modulate intramolecular charge transfer (ICT) strength and frontier molecular orbital hybridization. This achieves targeted absorption peaks at 621 nm (AzBdpy-B), 735 nm (AzBdpy-G), and 535 nm (AzBdpy-R), respectively. The incorporation of azulene not only enables broad spectral tunability but also effectively suppresses radiative decay, resulting in near-zero visible fluorescence—critical for minimizing background luminance in CFs. CFs fabricated from these materials demonstrate good photothermal stability (ΔEab < 3 after 150°C heating and UV exposure), high color purity, and wide sRGB coverage (81%), with photolithographic resolution down to 8.2-10.7 µm. Combined experimental and theoretical analyses—including single-crystal X-ray diffraction, hole-electron distribution, and Independent Gradient Model (IGM)—reveal how azulene-BODIPY electronic coupling governs both optical performance and structural robustness. This work establishes azulene-functionalized BODIPYs as a promising platform for high-resolution, low-emissivity RGB color photoresists, offering new insights into the molecular engineering of advanced dye-based optoelectronic materials.
Aggregation-induced emission (AIE) is a powerful route to amplify weakly emissive metal nanoclusters, yet simultaneously achieving AIE, structural precision, and ink compatibility remains challenging. Here, we demonstrate an aldehyde-functional cellulose ether as a soft, switchable template that regulates aggregation and emission of Ag6-derived cluster species. Periodate oxidation converts hydroxypropyl methylcellulose (HPMC) into dialdehyde HPMC (DHPMC), which forms swollen, homogeneous domains in water but collapses into confining microenvironments in ethanol-rich media. In the presence of 2-mercaptonicotinic acid (H2 mna), DHPMC promotes the formation of Ag6-derived cluster species; the corresponding Ag6(H2mna)6 crystalline core is established in the crystalline state by single-crystal X-ray diffraction, while negative-mode ESI-MS supports the presence of Ag6-derived species in solution. Notably, DHPMC converts inefficient aggregation into emissive aggregation. In 85 vol% ethanol, DHPMC/H2mna@AgNCs shows a dominant emission at 578 nm (λex = 385 nm), a quantum yield of 1.70%, and an average lifetime of 63.64 ns, reflecting suppressed non-radiative decay in a microenvironment-sensitive excited state. Structural and microscopic analyses further indicate that, in the presence of H2 mna, the DHPMC-containing formulations favor cluster-derived Ag-containing domains rather than plasmonic Ag nanoparticles. Coupled with printing-adapted rheology and antibacterial performance, this platform enables fluorescent patterns and latent fingerprint visualization, providing a practical polymer-cluster co-design strategy for multifunctional security inks.
Oncolytic virotherapy represents a compelling strategy for cancer immunotherapy, integrating direct tumor cell lysis with the activation of systemic antitumor immunity. Despite its therapeutic promise, clinical translation remains fundamentally limited by inefficient viral delivery, rapid immune clearance, and the highly immunosuppressive tumor microenvironment (TME). These barriers have shifted the field from virus-centric optimization alone toward integrated engineering strategies that jointly modulate viral design, delivery platforms (e.g., cell-based, microbial, or engineered systems), and host immunity. This review examines how genetic engineering has improved the potency and selectivity of oncolytic viruses (OVs) under local administration, and how delivery platforms have expanded these capabilities by enabling viral protection, controlled release, and microenvironmental modulation. In addition, emerging strategies for systemic delivery, including molecular camouflage, carrier-mediated transport, and biomimetic nanosystems designed to overcome immune neutralization and enhance tumor targeting, are discussed. Finally, we outline key design principles for the next generation of oncolytic virotherapy, emphasizing the need for spatiotemporally controlled, immune-integrated delivery systems that can support safe and effective systemic treatment.
Short-wavelength infrared (SWIR) organic light-emitting diodes (OLEDs) are highly attractive for applications in night vision, bio-imaging, and optical communication, yet achieving efficient emission beyond 900 nm remains challenging due to severe non-radiative losses and limited exciton utilization. Here, we introduce a phosphorescent-host-based exciton management strategy, in which phosphorescent materials function as hosts rather than conventional sensitizers. By simultaneously harvesting singlet and triplet excitons, this approach enables highly efficient SWIR OLEDs with an emission peak at 1000 nm. The resulting devices deliver a record external quantum efficiency (EQE) exceeding 0.22% and a radiance of 1805 mW sr−1 m−2, representing record performance for SWIR OLEDs. Photophysical studies reveal that host-mediated exciton management and triplet energy confinement are critical to suppressing energy-loss pathways. This work establishes a general host-engineering strategy for extending OLED emission into the SWIR region.
The integration of precise diagnosis with mechanism-based therapy remains a pivotal challenge in colorectal oncology. Here, building on the triphenylamine (TPA) core, we employed a donor‒acceptor (D‒A) molecular design strategy by integrating a pyridinium acceptor to engineer TPA-FB, a derivative exhibiting aggregation-induced emission (AIE) characteristic. Both in vitro and in vivo experiments demonstrated that TPA-FB functioned as an effective theranostic agent against colorectal cancer (CRC). Prompted by its molecular structure and notable biological activity, we sought to identify its specific cellular target. We discovered that TPA-FB directly binds to and inhibits the phosphorylation of STAT3, leading to downregulation of SUCLG2. Suppression of SUCLG2 thereby disrupts the tricarboxylic acid (TCA) cycle, reducing succinate and its downstream metabolites, which also disrupts critical protein succinylation modifications. By employing our designed AIEgen to selectively disrupt the STAT3‒SUCLG2 axis, we offer a transformative perspective for the development of CRC therapeutics.