Antimicrobial peptides (AMPs) have attracted great attention over the past few years as promising candidates to combat bacterial resistance. However, their small molecule nature poses limitations in stability, toxicity, and pharmacokinetics, restricting their in vivo and clinical uses. Supramolecular assembly of AMPs into well-defined nanostructures displays great potential to address the faced challenges, exhibiting unprecedented advantages over the unimolecular ones. The nanostructured AMPs could amplify therapeutic outcomes through enhanced germicidal capacity, improved serum stability, increased host compatibility and prolonged circulation. More importantly, through rational design, one can effectively modulate the interactions between peptides and microbes, promoting capabilities for bacterial capturing, and membrane targeting and disruption. In this review, the recent progress of supramolecular peptide assemblies as antimicrobial materials will be discussed with a focus on the design principle, self-assembly behavior, and applications of supramolecular AMPs. This supramolecular platform could provide excellent alternatives towards traditional antibiotics and AMPs, offering new solutions to tackle drug-resistant infectious pathogens.

Viologens exhibit reversible redox properties and remarkable color response, making them core materials in electrochromism. However, their low conjugation compromises charge transfer efficiency, undermines redox reversibility, and causes fluorescence quenching, thereby limiting their applications. This study addresses this challenge by proposing a synergistic design strategy of 'aromatic bridging-flexible side chains.' Incorporating electron-rich carbazole groups into the viologen backbone as a rigid bridging structure expands the molecular conjugation network; while tuning the length of the alkyl side chains on both sides suppresses molecular aggregation. Following this strategy, we designed and synthesized carbazole-viologen derivatives substituted with hydroxypropyl (HICDP) and hydroxyhexyl (HICDH) groups. A systematic investigation revealed how the carbazole unit and side-chain length regulate their electrochromic and photoluminescent properties. Experiments showed that the carbazole bridging unit expanded the conjugation system, enabling HICDH to achieve an optical contrast of Delta T = 77.4 % at 700 nm. Even after 100 cycles, HICDH retained approximately 70 % of its optical contrast. The increased side-chain length in carbazole-viologen derivatives increased the distance between radicals, suppressed dimer formation, and enhanced stability. Meanwhile, the material exhibited excellent photoluminescent properties. Theoretical calculations further confirmed that the side-chain extension strategy suppressed radical dimerization through steric hindrance. The hexyl side chain reduced the HOMO-LUMO bandgap to facilitate electron transitions while increasing the molecular dihedral angle to minimize non-radiative recombination. The extension of the side chains effectively suppressed non-radiative transition pathways, ultimately enhanced both the photochromic and electrochromic performance.

Supramolecular peptide hydrogels (SPHs), a unique class of dynamic three-dimensional networks formed by self-assembly of peptides, have demonstrated strong potential for ocular tissue replacement and drug delivery in ophthalmic applications. On the one hand, their mechanical and physiochemical properties can be precisely tailored via rational design of peptides to emulate native ocular tissues. On the other hand, the intrinsic dynamic features of SPHs enable efficient encapsulation of commercial drugs and incorporation of stimuli-responsive or targeting moieties, which in turn facilitate ocular barrier penetration and enhance therapeutic efficacy. In this review, we systematically summarize recent advances of the use of SPHs in ocular disease treatment, focusing on their design principles and two key application aspects: ocular tissue substitutes (for vitreous and corneal repair) and drug delivery systems targeting prevalent ocular pathologies, including dry eye disease, corneal neovascularization, bacterial keratitis, anterior uveitis, diabetic retinopathy, and age-related macular degeneration. These findings highlight the promising potential of SPHs as next-generation biomaterials for precision ophthalmic therapy.

The development of large-scale, high-fidelity quantum processors is a fundamental scientific challenge, essential for exploring the boundaries of classical computation and advancing towards fault-tolerant systems. Gaussian boson sampling not only serves as a prominent model for demonstrating quantum computational advantage1-3 but can also generate bosonic error-correcting codes for fault-tolerant quantum computing4-6. However, its scalability has been hindered by significant photon loss in increasingly large and complex encoding circuits. Here we show a programmable photonic quantum processor, Jiuzhang 4.0, which incorporates 1,024 high-efficiency squeezed states into a hybrid spatial-temporal encoded 8,176-mode circuit. By achieving 92% source efficiency and 51% overall system efficiency, the processor produces samples with detection events up to 3,050 photons, representing an order-of-magnitude increase in scale over previous demonstrations7-10. This architecture realizes a cubic scaling of connectivity (163 = 4, 096), enabling sampling within a Hilbert space of dimension approximately 102,461. The experimental results are rigorously validated against all current classical simulation methods, especially the matrix product state algorithms recently designed to exploit photon loss11. The ability to control thousands of photons in programmable low-loss quantum processors pushes the experimental frontier into a regime far beyond classical tractability and opens a pathway to trillion-qumode three-dimensional cluster states and fault-tolerant photonic quantum hardware.

Gaussian boson sampling (GBS) is one of the leading approaches for demonstrating quantum computational advantage, but its application to practical real-world problems remains a central challenge. Here, we propose a GBS-based image recognition scheme inspired by extreme learning machine to enhance the performance of perceptron and implement it using our latest GBS device, jiǔzhāng 4.0. By avoiding in situ programmability of the photonic circuit, the scheme substantially reduces experimental overhead while retaining a large, fixed random feature map. Our approach utilizes an 8176-mode temporal-spatial hybrid encoding photonic processor, achieving approximately 2200 average photon clicks in the quantum computational advantage regime. We apply this scheme to classify images from the MNIST and Fashion-MNIST datasets, achieving a testing accuracy of 95.86% on MNIST and 85.95% on Fashion-MNIST, respectively. These results surpass both classical linear-kernel support vector machines and the three previous physical extreme-learning-machine experiments. In addition, we systematically explore the influence of three key hyperparameters and the efficiency of GBS in our experiments. Our results not only demonstrate the potential of GBS in real-world machine learning applications but will also inspire further advancements in powerful machine learning schemes utilizing GBS technology.

Biomolecular condensates formed via liquid-liquid phase separation function as dynamic organelles that are vital to regulating cellular activities. Peptide-based coacervates have emerged as appealing candidates to resemble key properties of biomolecular condensates. However, their application as adaptive organelles has been hindered by structural complexity and limited control over phase-separation. Here, we present short tripeptide coacervates with tunable phase-separation behaviors governed by composition and peptide sequence, significantly reducing molecular complexity. These tripeptide condensates exhibit enzyme-regulated phase-separation, closely mimicking the dynamic nature of biomolecular condensates. A key attractive feature of the tripeptide coacervates is their capability to sequester both hydrophobic active species and hydrophilic enzymes. This unique property enables the execution of confined tandem reactions in aqueous conditions. When incorporated into membrane-bound artificial cells, this tripeptide coacervates serve as adaptive sub-organelles, orchestrating compartmentalized catalytic cascades. This work highlights the potential of minimalistic peptide systems as functional microreactors with biomimetic and catalytic capabilities.

The formation of active and catalytic biomolecular condensates is critical to orchestrate intracellular biochemical reactions and cellular functions. Synthetic analogues that mimic such behaviors are typically constructed via liquid-liquid phase separation that generates liquid coacervate-based droplets, which promote reaction efficiency through molecular confinement. Such a type of confined reaction is usually achieved by partitioning and sequestrating active species such as biological enzymes or their mimics (such as metalloenzymes), which can be easily affected by encapsulation efficiency and sensitivity to the local environment. Engineering coacervate-based compartments that can display inherent catalytic functionality remains a significant challenge. Here, we report a bioinspired strategy to construct programmable peptide-based coacervates with inherent enzyme-like catalytic activity via the co-assembly of short peptides. We find that mixing the histidine-tagged short peptides with triphenylalanine-based peptides leads to the formation of a stable coacervate phase, in contrast to the rigid aggregates formed by each individual component. This cooperative assembly enables the generation of functional coacervate compartments with built-in catalytic capability. The resulting peptide coacervates exhibit selective partitioning and sequestration of hydrophobic substrates, thereby enhancing local substrate concentration and promoting catalytic hydrolysis reactions. Our results demonstrate that catalytic activity can be encoded directly into coacervate-forming building blocks through rational peptide design, providing a versatile platform for programming LLPS behavior and constructing biomimetic active materials with potential applications in synthetic biology.

Phosphorescence-based oxygen sensors offer an efficient route to rapid oxygen visualization, yet their practical deployment is often hindered by nonlinear Stern-Volmer responses and low sensitivity arising from heterogeneous microenvironments in physically mixed systems. Here, we report a scalable morphological-engineering strategy to construct microporous films with room-temperature phosphorescence (RTP) that show ultralinear oxygen sensing. Triphenylamine-derived phosphors are covalently integrated into amphiphilic copolymers composed of hydrophobic and hydrophilic segments, effectively suppressing phosphor aggregation. By judiciously selecting volatile nonazeotropic and azeotropic mixed solvents, we direct the formation of interconnected microporous networks or perforated microcells, thereby dramatically increasing the quenchable phosphorescent fraction. The resulting films exhibit long RTP lifetimes (∼100 ms) and ultralinear oxygen sensing (R2 > 0.999) with Stern-Volmer quenching constants KSV of up to 2071, together with excellent reproducibility. These afterglow microporous films further enable real-time visualization of gas flow and underwater dissolved oxygen monitoring, demonstrating their potential as reliable platforms for high-performance oxygen sensing.

Abstract Substitutions at the nodal and anti-nodal positions of conjugated aromatics exert profound effects on their electronic properties, yet a systematic investigation is lacking on how these underlying quantum mechanical rules are manifested experimentally. Here, using polycyclic aromatic hydrocarbons derivatives as a model system, we systematically elucidate how nodal and anti-nodal substitutions dictate their chemical reactivity and physical properties. It is found that Sonogashira C–C coupling at the nodal position has a noticeably lower product yield than anti-nodal position under identical reflux conditions due to inhibited molecular orbital amplitude. Comprehensive spectroscopic characterization of the resulting substituted products reveals two striking photophysical differences: 1) Frontier orbital symmetry is largely conserved in node-substituted molecules, whereas the anti-nodal substitution induces strong symmetry-breaking, leading to accelerated fluorescence emission in anti-node-substituted pyrenes; 2) Nodal substitution induces the formation of charge-transfer states due to a twisted geometry, which activates room-temperature phosphorescence via improved singlet–triplet intersystem crossing. This study establishes an effective structure–property relationship linking molecular orbital symmetry to macroscopic cross-coupling reactivity and molecular photophysics within these conjugated aromatics.

Organic electrochromic materials have shown considerable potential for applications in smart windows, biosensors, and energy-storage devices owing to their tunable molecular structures, facile preparation, and rich color variation. Conventional viologen compounds are susceptible to over-reduction in their reduced states, which induces irreversible structural changes and limits their application in bifunctional electrochromic-photoluminescent devices. Viologen molecules possess excellent structural designability, and their optical and electrochemical properties can be precisely modulated by modifying substituent structures, counterions, and conjugation lengths, giving them irreplaceable advantages in electrochromic applications. In this study, an aromatic-bridging strategy was adopted, in which dibenzo[b,d]thiophene and dimethoxybenzene units were introduced between pyridine rings to modulate molecular conjugation and charge transport, while hydroxyhexyl side chains were incorporated to improve molecular solubility and intermolecular interactions. The experimental results demonstrate that the successfully prepared 4,4′-(2,5-dimethoxy-1,4-phenylene)bis(1-(6-hydroxyhexyl)pyridin-1-ium) dibromide (DMBBH) exhibits outstanding performance. DMBBH enables a reversible transition from a transparent state to a deep-red state, with an optical contrast of ΔT = 72.0%, a high coloration efficiency of η = 183.90 cm2/C, coloration (τc)/bleaching (τb) response times of 9.5 s and 51 s, respectively, and an optical contrast that remains at 61.8% after 10000 s of cycling. This work demonstrates the key role of aromatic bridging structures in stabilizing the excited states of viologen molecules and optimizing charge-transport pathways, providing a new design strategy for future high-performance bifunctional organic optoelectronic devices.

Spontaneous association of multiple components into coassemblies significantly amplifies the complexity of supramolecular systems. Owing to varied noncovalent interactions, the precise regulation of the copolymerization pathway, molecular arrangement, and assembled morphology remains a huge challenge. Here, we report an intriguing system as the first example of using complementary stereocomplexation between enantiomeric oligo(lactic acid)s (oLAs) to govern the supramolecular copolymerization behavior of a series of amphiphilic peptide conjugates. Specifically, the hydrophobic chiral oLAs were conjugated to various peptides, which can self-assemble on their own in an aqueous environment into straight nanofibers with bilayer molecular packing. Upon copolymerization between two monomers with enantiomeric oLAs, helical filamentous nanostructures with an interdigitated bilayer molecular arrangement were observed. A combination of TEM imaging and spectroscopic analysis further revealed the formation of alternating microstructures in the supramolecular copolymers under thermodynamic equilibrium, promoted via stereospecific interactions between enantiomeric hydrophobic chains. In addition, the copolymerization can shift from a stereocomplexation-driven to a hydrogen-bonding-dominated process with the increase in β-sheet-forming propensity in peptides, exhibiting similar self-assembly behaviors to their homopolymer counterparts. We believe that these findings provide a new perspective on the formation of alternating supramolecular copolymers and modulation between multiple intermolecular interactions.

Artificial intrinsically disordered proteins (IDPs) are often biosynthesized in cells by repeating low-complexity sequences derived from native IDPs through rational engineering. Herein we report the chemical synthesis of stereocontrolled linear and cyclic IDP mimics with up to 640 amino acids (∼52 kDa) via an iterative exponential growth (IEG) strategy. Following a known sequence originating from the disordered region of natural tropoelastin, linear elastin-like polypeptides (ELPs) were synthesized by conjugating monomeric pentapeptides via IEG, which transferred the sequence and chiral features of pentapeptides to the resultant polypeptides, thereby achieving robust control of their molecular weights and stereochemistry. Cyclic ELPs with different molecular weights were further synthesized via intramolecular amidation. Distinct lower critical solution temperature phase transition behaviors were observed with varying molecular weights, stereochemistry, and topology of ELPs. Our work demonstrates a new synthetic route toward chemically complex ELPs and the profound impact of chemical parameters on their properties.

The creation of large-scale, high-fidelity quantum computers is not only a fundamental scientific endeavour in itself, but also provides increasingly robust proofs of quantum computational advantage (QCA) in the pres- ence of unavoidable noise and the dynamic competition with classical algorithm improvements. To overcome the biggest challenge of photon-based QCA experiments, photon loss, we report new Gaussian boson sampling (GBS) experiments with 1024 high-efficiency squeezed states injected into a hybrid spatial-temporal encoded, 8176-mode, programmable photonic quantum processor, Jiuzhang 4.0, which produces up to 3050 photon de- tection events. Our experimental results outperform all classical spoofing algorithms, particularly the matrix product state (MPS) method, which was recently proposed to utilise photon loss to reduce the classical simula- tion complexity of the GBS. Using the state-of-the-art MPS algorithm on the most powerful supercomputer EI Capitan, it would take > 1042 years to construct the required tensor network for simulation, while our Jiuzhang 4.0 quantum computer takes 25.6 μs to produce a sample. This work establishes a new frontier of QCA and paves the way to fault-tolerant photonic quantum computing hardware.

Bonding aromatic ring to carbonyl group is recognized as crucial for promoting intersystem crossing (ISC) owing to allowed 1 nπ* → 3 ππ* or 1 ππ* → 3 nπ* transition. The effect of charge transfer (CT) in such systems, however, is largely ignored for understanding ISC and phosphorescence efficiency. Here, we unveiled a principle for producing highly‐efficient room‐temperature phosphorescence (RTP) polymer where the role of CT in diarylketone phosphors was a prerequisite. Designed diarylketones with carbonyl group substituted by aromatic rings unsymmetrically achieved superior RTP quantum yield of >30% in copolymer. Detailed investigation indicated that 1 CT→ 3 LE (locally excited triplet state) transition with small energy gap (∆ E ST ) and strong spin‐orbit coupling underlies their ultrafast ISC, as recorded by femtosecond transient absorption (fs‐TA) spectroscopy. When single aromatic ring was bonded to carbonyl group, singlet (S 1 ) and triplet (T 1 ) states remained LE with large ∆ E ST and weak spin‐orbit coupling, leading to low RTP efficiency. Finally, manufacturing organic glass in presence of trace diarylketone monomers could generate shape‐rich three‐dimensional (3D) objects with intense afterglow under room lighting, even at high‐temperature and wet conditions. This work advances understanding on structure‐property relationship in popular aromatic ketone phosphors, and paves the way for producing afterglow materials with high brightness and stability.

Freezing-induced enrichment of organic solutes within ice has long been hypothesized to play a pivotal role in prebiotic chemistry and the origins of life, yet direct evidence for the in-ice aggregation of dilute, water-soluble organics has remained elusive. Here, we employ a conformation-sensitive organic phosphor, 2-phenylbenzothiazole iodide (SNI), to uncover the formation of amino-acid nanoaggregates in water ice. Unusual, amino-acid-specific phosphorescence signatures from SNI-guided investigations prompted us to examine the frozen samples with cryo-transmission electron microscopy (cryo-TEM), which directly revealed uniform nanoaggregates. These nanoaggregates create distinct local microenvironments that influence photophysical properties of SNI, inducing distinct ground-state conformations that lead to conformation-dependent phosphorescence. Complementary theoretical calculations, molecular dynamics simulations, and temperature-variable Raman spectra suggest that amino acids, such as alanine, undergo a temperature-dependent proton-transfer process from their ammonium to carboxylate groups, enhancing their hydrophobicity and triggering aggregation upon freezing. This enrichment of amino acids in ice sets the stage for subsequent polymerization reactions, shedding new light on how primitive icy environments could have facilitated the emergence of peptide-based prebiotic chemistry.

Gaussian boson sampling (GBS) has emerged as a promising quantum computing paradigm, demonstrating its potential in various applications. However, most existing works focus on theoretical aspects or simple tasks, with limited exploration of its capabilities in solving real-world practical problems. In this work, we propose a novel GBS-based image recognition scheme inspired by extreme learning machine (ELM) to enhance the performance of perceptron and implement it using our latest GBS device, Jiuzhang. Our approach utilizes an 8176-mode temporal-spatial hybrid encoding photonic processor, achieving approximately 2200 average photon clicks in the quantum computational advantage regime. We apply this scheme to classify images from the MNIST and Fashion-MNIST datasets, achieving a testing accuracy of 95.86

Freezing-induced enrichment of organic solutes within ice has long been hypothesized to play a pivotal role in prebiotic chemistry and the origins of life, yet direct evidence for the in-ice aggregation of dilute, water-soluble organics has remained elusive. Here, we employ a conformation-sensitive organic phosphor, 2-phenylbenzothiazole iodide (SNI), to uncover the formation of amino-acid nanoaggregates in water ice. Unusual, amino-acid-specific phosphorescence signatures from SNI-guided investigations prompt us to examine the frozen samples with cryo-transmission electron microscopy (cryo-TEM), which directly reveals uniform nanoaggregates. These nanoaggregates create distinct local microenvironments that influence the photophysical properties of SNI, inducing distinct ground-state conformations that lead to conformation-dependent phosphorescence. Complementary theoretical calculations, molecular dynamics simulations, and temperature-variable Raman spectra suggest that amino acids, such as alanine, undergo a temperature-dependent proton-transfer process from their ammonium to carboxylate groups, enhancing their hydrophobicity and triggering aggregation upon freezing. This enrichment of amino acids in ice may represent a prerequisite condition for polymerization, offering new insights into how primitive icy environments could have influenced peptide-based prebiotic chemistry.

Probing quantum coherence in excitonic energy transfer (EET) is critical for understanding and designing advanced organic optoelectronic materials and devices. However, direct experimental evidence for coherent EET under ambient conditions remains elusive due to the complexity and losses inherent in molecular solids. Here, we demonstrate a straightforward steady-state photoluminescence spectroscopic approach that selectively probe coherent exciton populations in engineered organic doping systems. Using pyrene or anthracene derivatives as dopants (guest) within the crystal of a naphthalene derivative (host), the type of EET from the host to the guest is highly selective, governed by quantum coherence. Specifically, the coherent aggregate exciton population of the host is almost entirely depleted, whereas the host monomer emission largely persists in the presence of the guest dopant, despite the guest absorption being better matched to the host monomer emission. By chemically modifying the energy donor naphthalene, the populations of aggregate and monomer excitons of the host can be systematically tuned, which directly correlates with the sensitivity of the guest photoluminescence in doped host crystals. These findings have important implications for understanding exciton dynamics in optoelectronic devices.

Room-temperature phosphorescence (RTP) has extensive applications in various fields such as data encryption, chemical sensing, optoelectronic displaying, and time-resolved bioimaging, yet most materials are fossil fuel-based. Recently, an increasing interest has emerged with respect to natural organic RTP. However, the cases are rare and the structure-property relationships remain poorly understood. Here, natural nuts with prevalent RTP characters were unveiled with comprehensive elucidation on the molecular origins, representing an alternative reservoir of sustainable and clean RTP materials. The nuts generally show seconds-long afterglow at ambient conditions, relying heavily on excitation wavelengths and nut composition. RTP of intrinsic nutrients including aromatic vitamins, aromatic nucleobases, and aromatic amino acids dispersed in nonaromatic natural media at low contents (as low as the ppm level) covers the entire RTP spectra of nuts, spanning <400 to >700 nm. Different aromatic nutrients require varied excitation energies and are capable of showing distinct RTP colors. Thus, biomatrices and diverse aromatic nutrients should rationalize excitation-dependent broad-band nut RTP synergistically, both of which should not be overlooked. Furthermore, nut RTP can be facilely modulated by trace polyaromatic phosphors, facilitating color-tunable 3D afterglow for multilevel information storage. This work considerably expands the scope of natural RTP based on abundant sources and provides new insights into the underlying mechanism, opening a broad avenue for applying sustainable luminescent materials that can be produced at a large scale and low cost.

Complexation between two organic molecules can occur either for strong electron donor-acceptor pairs in the ground state, known as charge-transfer complexes (CTCs), or for pairs of lesser strength in the excited state, such as excimers and exciplexes. However, the characterization of chemically distinct CTCs in solution remains elusive. Here, we report a light-induced, solution-persistent 1:1 CTC between an amine and an imide. The pair is not associated in the ground state at room temperature prior to light exposure. The presence and exact molecular compositions of the CTCs could be directly obtained from high-resolution mass spectrometry. Additional spectroscopic and computational evidence reveal that a kinetically trapped ground-state pair is formed following an exciplex-like process between the amine and the imide after photoexcitation. We show that such a photoinduced complex can be used to conduct photochemistry and store photon energy for producing otherwise photochromic products in the dark.