Electrostatic Assembly of Gold Nanoclusters in Reverse Emulsion Enabling Nanoassemblies with Tunable Structure and Size for Enhanced NIR-II Fluorescence Imaging.

The precise control of the assembly structure and size of gold nanoclusters (AuNCs) can potentially amplify their near-infrared II (NIR-II) fluorescence imaging and targeting properties. However, the conventional electrostatic assembly of AuNCs and charged molecules faces challenges in balancing the inherent electrostatic repulsions among charged units and regulating the diffusion of assembly units. These difficulties limit precise control over assembly size and structure, along with limited options for coassembled molecules, thereby restricting imaging properties and targeting capability.

Surface Modification of Gold Nanorods: Multifunctional Strategies and Application Prospects.

Gold nanorods (AuNRs), as an important type of gold nanomaterials, have attracted much attention in the nano field. Compared with gold nanoparticls, AuNRs have broader application potential due to their tunable localized surface plasmon resonance properties and anisotropic shapes. Yet, conventional synthesis methods using surfactants have limited the use of AuNRs in a variety of fields such as biomedical applications, plasma-enhanced fluorescence, optics and optoelectronic devices.

Scalable production of structurally colored composite films by shearing supramolecular composites of polymers and colloids.

Structurally colored composite films, composed of orderly arranged colloids in polymeric matrix, are emerging flexible optical materials, but their production is bottlenecked by time-consuming procedures and limited material choices. Here, we present a mild approach to producing large-scale structurally colored composite films by shearing supramolecular composites composed of polymers and colloids with supramolecular interactions. Leveraging dynamic connection and dissociation of supramolecular interactions, shearing force stretches the polymer chains and drags colloids to migrate directionally within the polymeric matrix with reduced viscous resistance.

Decoding the Pathway-Dependent Self-Assembly of Polymer-Grafted Nanoparticles by Ligand Crystallization.

Functional metamaterials can be constructed by assembling nanoparticles (NPs) into well-ordered structures, which show fascinating properties at different length scales. Using polymer-grafted NPs (PGNPs) as a building block, flexible composite metamaterials can be obtained, of which the structure is significantly affected by the property of polymer ligands. Here, it is demonstrated that the crystallization of polymer ligands determines the assembly behavior of NPs and reveal a pathway-dependent self-assembly of PGNPs into different metastructures in solution.

Effect of Polymeric Ligand Grafting Region on Confined Assembly of Gold Nanorods in cylindrical nanopores.

The grafting region of polymeric ligands exhibit a significant influence on the assembly behavior of polymer tethered gold nanorods (AuNRs) in confined space. In this work, the effect of core size, molecular weight and grafting region of ligands on the assembly structure in cylindrical nanopores was investigated. It is found that polystyrene end-tethered AuNR (AuNR@End-PS) exhibits a dumbbell-like shape, while the AuNR with PS tethered on the entire surface (AuNR@Full-PS) shows a rod-like morphology that gradually transforms into a spherical shape as the molecular weight increases.

Electrostatically Controlled and Polymerization of Diacetylene-Containing Peptide Amphiphiles in Living Cells.

Precise control of diacetylene-containing peptide amphiphile (DPA) based supramolecular architectures is important for their polymerization behaviors and biomedical applications. Herein, we reported two DPAs (cationic PA-NH and zwitterionic PA-OH) with a similar molecular structure, which exhibited completely opposite polymerization behaviors in aqueous solution and living cells. Specifically, PA-NH was unpolymerizable in aqueous solution but underwent polymerization to respond to the intracellular microenvironment.

Fabrication of Oriented Colloidal Crystals from Capillary Assembly of Polymer-Tethered Gold Nanoparticles.

Self-assembled colloidal crystals (CCs) or nanoparticle (NPs) superlattices have attracted significant attention due to their potential applications in many fields. However, due to the complex interactions that govern the self-assembly, it is difficult to predict and control the superstructure organization of CCs. Herein, a facile yet effective way is demonstrated to fabricate oriented CCs from capillary assembly of polymer-tethered gold NPs (AuNPs).

Revealing the dynamic adsorption and diffusion of peptide amphiphile on supported lipid bilayer by single molecule experiment and simulation.

Dynamic adsorption and diffusion of peptide amphiphiles (PAs) with different numbers of alkyl tails on supported lipid bilayers (SLBs) were investigated by single molecule tracking experiment and molecule dynamic simulation. Experimental results show two distinct populations of PAs with different residence time. Residence time of adsorbed PAs increases with the increase of the alkyl tails, whereas diffusion coefficient monotonically decreases with rising the number of alkyl tails and also decreases with increasing the mobility of SLBs.

Self-Assembly of Polymer End-Tethered Gold Nanorods into Two-Dimensional Arrays with Tunable Tilt Structures.

We demonstrated a facile yet effective strategy for self-assembly of polymer end-tethered gold nanorods (GNRs) into tunable two-dimensional (2D) arrays with the assistance of supramolecules of hydrogen bonded poly(4-vinyl pyridine) (P4VP) and 3--pentadecylphenol (PDP). Well-ordered 2D arrays with micrometer size were obtained by rupturing the assembled supramolecular matrix with a selective solvent. The formation of long-range ordered 2D arrays during a drying process was observed via small-angle X-ray scattering.

Highly Luminescent Liquid Crystals in Aggregation Based on Platinum(II) Complexes.

Luminescent liquid crystals (LLCs) attract considerable attention because of their broad applications in displays, chemosensors, and anti-counterfeiting. However, it remains challenging to achieve a high luminescence efficiency in LCs because of the common aggregation-caused quenching effect. Herein, we demonstrate a facile approach to designing LLCs with a high quantum yield up to 88% by deliberately tuning the aggregation behavior of platinum(II) complexes with alkoxy chains (CHO-).

Lipidated gemini peptide amphiphiles with enhanced loading capacity and cell membrane affinity for drug delivery.

Lipidated peptide amphiphiles exhibit high affinity for plasma cell membranes, good cell internalization and improved stability against degradation, which make them attractive as a drug delivery system. However, low drug loading capacity limits their application for drug delivery. Herein, we developed a gemini peptide amphiphile with enhanced membrane activity and endosomal escape, containing dodecanoic acid hydrophobic tails at the N-terminus, rhodamine on the pendant chain and an active targeting peptide sequence (GRGDS).

Dopant-Free Crossconjugated Hole-Transporting Polymers for Highly Efficient Perovskite Solar Cells.

Currently, there are only very few dopant-free polymer hole-transporting materials (HTMs) that can enable perovskite solar cells (PVSCs) to demonstrate a high power conversion efficiency (PCE) of greater than 20%. To address this need, a simple and efficient way is developed to synthesize novel crossconjugated polymers as high performance dopant-free HTMs to endow PVSCs with a high PCE of 21.3%, which is among the highest values reported for single-junction inverted PVSCs.

Tunable Photonic Microspheres of Comb-Like Supramolecules.

Photonic crystals (PCs) are ideal candidates for reflective color pigments with high color purity and brightness due to tunable optical stop band. Herein, the generation of PC microspheres through 3D confined supramolecular assembly of block copolymers (polystyrene-block-poly(2-vinylpyridine), PS-b-P2VP) and small molecules (3-n-pentadecylphenol, PDP) in emulsion droplets is demonstrated. The intrinsic structural colors of the PC microspheres are effectively regulated by tuning hydrogen-bonding interaction between P2VP blocks and PDP, where reflected color can be readily tuned across the whole visible spectrum range.

Diffusion behavior of peptide amphiphiles containing different numbers of alkyl tails at a hydrophobic solid-liquid interface: single molecule tracking investigation.

Using the single molecule tracking technique, the diffusion behavior of peptide amphiphiles (PAs) with different numbers of alkyl tails at a hydrophobic solid-liquid interface has been investigated. The effect of the number of alkyl tails of PAs on molecular trajectories at the hydrophobic solid-liquid interface has been systematically studied. PA molecules display an intermittent motion consisting of immobilization and hopping processes, which has been well simulated by the continuous time random walk (CTRW) model.

Construction of Supramolecular Liquid-Crystalline Metallacycles for Holographic Storage of Colored Images.

Design and construction of new functionalized supramolecular coordination complexes (SCCs) via coordination-driven self-assembly strategy is highly important in supramolecular chemistry and materials science. Herein, we present a family of well-defined metallacycles decorated with mesogenic forklike dendrons through the strategy of coordination-driven self-assembly. Due to the existence of mesogenic forklike dendrons, the obtained metallacycles displayed the smectic A liquid crystal phase at room temperature while their precursors exhibited the rectangular columnar liquid crystal phase.

Reversible photo-responsive gel-sol transitions of robust organogels based on an azobenzene-containing main-chain liquid crystalline polymer.

Stimuli-responsive supramolecular gels have been widely investigated, but the construction of a liquid crystalline gel with a high mechanical property and reversible photo-response still remains a challenge. This is due to the difficulty of designing gelators with liquid crystal properties and gelation abilities in organic solvents simultaneously. In this study, an azobenzene-containing main-chain polyester (Azo-mLCP) with a pendant amide group was synthesized.

Dopant-Free Squaraine-Based Polymeric Hole-Transporting Materials with Comprehensive Passivation Effects for Efficient All-Inorganic Perovskite Solar Cells.

Development of high-performance dopant-free hole-transporting materials (HTMs) with comprehensive passivation effects is highly desirable for all-inorganic perovskite solar cells (PVSCs). Squaraines (SQs) could be a candidate for dopant-free HTMs as they are natural passivators for perovskites. One major limitation of SQs is their relatively low hole mobility.

Moebius strips of chiral block copolymers.

The Moebius topology (twisted, single-sided strip) is intriguing because of its structural elegance and distinct properties. Here we report the generation of block copolymer Moebius strips via a fast self-assembly of chiral block copolymer polystyrene-block-poly(D-lactide acid) (PS-b-PDLA) in tetrahydrofuran/water mixed solvents. The Moebius strip is formed by morphological evolution from large compound micelle (LCM) to spindle-like micelle (SLM) and then to toroid with a 180° twist along the ring.

Visible light-triggered gel-to-sol transition in halogen-bond-based supramolecules.

Photoresponsive supramolecular gels have aroused continuous attention because of their extensive applications; however, most studies utilize UV light, which inevitably brings about some health and environmental issues. The halogen bond is an important driving force for constructing supramolecules due to its high directionality, tunable strength, good hydrophobicity, and large size of the halogen atoms. Yet, it still remains a formidable challenge to utilize halogen bonds as a driving force to fabricate a visible light responsive gel.

Metallosupramolecular Photonic Elastomers with Self-Healing Capability and Angle-Independent Color.

Photonic elastomers that can change colors like a chameleon have shown great promise in various applications. However, it still remains a challenge to produce artificial photonic elastomers with desired optical and mechanical properties. Here, the generation of metallosupramolecular polymer-based photonic elastomers with tunable mechanical strength, angle-independent structural color, and self-healing capability is reported.