Lingxiang Jiang

South China University of Technology | SCUT · School of Molecular Science and Engineering

Proteins can readily assemble into rigid, crystalline and functional structures such as viral capsids and bacterial compartments. Despite ongoing advances, it is still a fundamental challenge to design and synthesize protein-mimetic molecules to form crystalline structures. Here we report the lattice self-assembly of cyclodextrin complexes into a v...

Polymer networks are fundamental from cellular biology to plastics technology but their intrinsic inhomogeneity is masked by the usual ensemble-averaged measurements. Here, we construct direct maps of crosslinks-symbolic depiction of spatially-distributed elements highlighting their physical features and the relationships between them-in an actin n...

The radial geometry with rays radiated from a common core occurs ubiquitously in nature for its symmetry and functions. Herein, we report a class of synthetic asters with well-defined core-ray geometry that can function as elastic and radial skeletons to harbor nano- and microparticles. We fabricate the asters in a single, facile, and high-yield st...

Due to the intrinsic lack of spatial order and self‐supported shape, liquids are often incompatible with precision manufacturing/processing and are potentially limited for advanced functionality. Herein, we develop an optothermal strategy to fully command phase‐separated liquids with unprecedent spatiotemporal addressability. Specifically, we focus...

Many soft tissues are compression-stiffening and extension-softening in response to axial strains, but common hydrogels are either inert (for ideal chains) or tissue-opposite (for semiflexible polymers). Herein, we report a class of astral hydrogels that are structurally distinct from tissues but mechanically tissue-like. Specifically, hierarchical...

Optical manipulation has emerged as a pivotal tool in soft matter research, offering superior applicability, spatiotemporal precision, and manipulation capabilities compared to conventional methods. Here, an overview of the optical mechanisms governing the interaction between light and soft matter materials during manipulation is provided. The dist...

It is an ongoing endeavor in chemistry and materials science to regulate coacervate droplets on a physiologically relevant spatiotemporal scale to ultimately match or even surpass living cells' precision, complexity, and functionality. Herein, we develop a magnetic strategy orthogonal to the thermal, pH, light, or chemical counterparts that are com...

Transport of rodlike particles in macromolecular networks is critical for many important biological processes and technological applications. Here, we report that speeding-up dynamics occurs once the rod length L reaches around integral multiple of the network mesh size ax. We find that such a fast diffusion follows the sliding dynamics and demonst...

At the very heart of any polymer networks are the crosslinks that interconnect neighboring chains and lock them in position to resist stress. The crosslinks and their spatial heterogeneity are expected to dictate network architecture, origin of elasticity, and transmission from macroscopic forces to local responses. Yet, direct confirmations of the...

Liquid Sculpture In article number 2205563, Yuchao Li, Lingxiang Jiang, and co‐workers present an optothermal strategy to dynamically control phase‐separated liquids with an unprecedented level of spatiotemporal addressability, for the realization of liquid painting and liquid animation, such as a liquid sculpture of a butterfly.

There is a fundamental gap between the inherent complexity of biology and the simplicity that physicists and chemists often seek. In this Perspective, we reason that liquid-liquid phase separation (LLPS) could be utilized to (partially) fill this gap and to bridge different disciplines because LLPS can produce condensed droplets with simplicity and...

Originated from supramolecular chemistry, the host-guest concept is generalized and appreciated across the fields of enzyme catalysis, biological channel conduction, and carbon nanotube transport, to name a few. Despite the extensive study of host-guest thermodynamics, it is still a fundamental challenge to directly measure its dynamics in real-spa...

A common practice to regulate surface energy (γ) depends on stimuli-responsive surfactants that switch between active and inactive forms; this equilibrium-based strategy is, however, binary in origin and difficult to...

If there is a secret recipe that enables living cells to build themselves from individual molecules, it is likely the hierarchical self-organization. Here, we summarize recent progress in the synthetic self-assembly analogous to subcellular structures, including flattened sacs, crystalline membranes, reconfigurable coacervate droplets, semiflexible...

Biomaterials in nature often exhibit hierarchical chiral structures with an intriguing mechanism involving hierarchical chirality transfer from molecular to supramolecular and the nano- or micro-scale level. To mimic the cross-level chirality transfer, we present here one kind of host-guest complex system built of β-cyclodextrin (β-CD), sodium dode...

We report that under mechanical pressure, caking of the precipitated molecular self-assemblies may lead to bulk supramolecular films. Massive fabrication of supramolecular films becomes possible using a simple household noodle machine. The film can be endowed diversified functions by depositing various functional ingredients via co-precipitation.

It is notoriously difficult to adhere water‐rich materials such as hydrogels and biological tissues. Existing adhesives usually suffer from weak and unadjustable adhesion strength partially because the contact between adhesives and substrates is largely restrained to the adhesive/substrate interface. Here, we approach this challenge by developing a...

While lipids form soft, fluidic membranes (soft assembly), proteins can readily assemble into rigid, crystalline structures such as viral capsids and bacterial compartments (lattice assembly). The key difference has to do with the driving forces, where the former is driven by the weak, directionless hydrophobic effect and the latter, by a combinati...

Stimulated emission depletion nanoscopy and its derivatives based on saturation induced competition effects have become an indispensable tool for studying cellular events and their dynamics in living conditions. The successful implementation of these techniques heavily relies on the competition between excitation induced spontaneous emission and st...

Utilizing a distinctly different approach from conventional fluorescent stimulated emission depletion (STED) nanoscopy, Xiangping Li and co‐workers (article number 1800432) demonstrate multiplexed fluorescence‐free superresolution imaging of gold‐nanoparticle labeled tumor cells. The superiority of this method in non‐bleaching, high resolution, and...

Caking of powder materials is undesired in various industries, and for thousands of years people are fighting against caking. Herein, the principle of caking is employed to create macroscopic plastic supramolecular films through a cold sintering process. A nanometer‐sized, irregular coordinating cluster is first generated with a bulky head surfacta...

In article number 1803370, Yun Yan and co‐workers employ the often undesired tendency of powders for caking to create macroscopic plastic supramolecular films. Upon exposing a powder, formed by coordinating clusters, to moisture under finger pressure, instantaneous congealing into a transparent film occurs. The resulting material is as strong as co...

Water in oil emulsions would be prepared by silicones (SO), modified silicones (DC8500) and a food-grade stabilizer (starch 1). With increasing water contents, the emulsions turned from a liquid-like to gel-like behaviors with enhancing storage and loss modulus. When DC8500/SO was 1/17 with 10 wt% starch 1, a high internal phase emulsion can be obt...

Noble metal nanoparticles (NPs), owing to their unique optical and physicochemical properties, are routinely used for optical imaging and labeling of biological specimens. Even though they can provide vital information for studying multiple cellular events and their interplays at the same time, optically multiplexing and resolving specific NPs with...

Supplementary Figures, Supplementary Discussion and Supplementary References

The key to spontaneous and directed assembly is to encode the desired assembly information to building blocks in a programmable and efficient way. In computer graphics, raster graphics encodes images on a single-pixel level, conferring fine details at the expense of large file sizes, whereas vector graphics encrypts shape information into vectors t...

Particle diffusion on colloidal monolayer without optical tweezers.

Thermal fluctuations of a colloidal arene.

Entanglement in polymer and biological physics involves a state in which linear interthreaded macromolecules in isotropic liquids diffuse in a spatially anisotropic manner beyond a characteristic mesoscopic time and length scale (tube diameter). The physical reason is that linear macromolecules become transiently localized in directions transverse...

The hierarchical self-assembly of sugar and surfactant molecules into hollow tubular microstructures was characterized in situ with high resolution small-angle X-ray scattering spanning more than three orders of magnitude of spatial scales. Scattering profiles reveal that aqueous host-guest inclusion complexes self-assemble into multiple equally sp...

Significance Highly entangled biofilaments are ubiquitous in the cytoskeleton and present a paradigm in polymer physics and biophysics. Here, rather than conventionally seeking to understand the self-diffusion of a single tagged entangled polymer we inquire into dynamic cross-correlations between nearby filaments as they diffuse anisotropically in...

We characterize the porosity of hydrogels by imaging the displacement trajectories of embedded tracer particles. This offers the possibility of characterizing the size and projected shape of individual pores as well as direct, real-space maps of heterogeneous porosity and its distribution. The scheme shows that when fluorescent spherical particles...

The spatially resolved diffusive dynamic cross correlations of a pair of colloids in dense quasi-two-dimensional monolayers of identical particles are studied experimentally and theoretically at early times where motion is Fickian. In very dense systems where strong oscillatory equilibrium packing correlations are present, we find an exponential de...

The paper is published in Part. & Part. Syst. Charact., 32, 313-320 (2015). Anisotropic and binary colloids self-assemble into a variety of novel supracolloidal structures within the thermo-switchable confi nement of molecular microtubes, achieving structuring at multiple length scales and dimensionalities. The multistage self-assembly strategy inv...

Anisotropic and binary colloids self-assemble into a variety of novel supracolloidal structures within the thermo-switchable confinement of molecular microtubes, achieving structuring at multiple length scales and dimensionalities. The multistage self-assembly strategy involving hard colloidal particles and a soft supramolecular template is generic...

The paper is available here: http://www.uu.nl/en/files/1790pdf Anisotropic and binary colloids self-assemble into a variety of novel supracolloidal structures within the thermo-switchable confinement of molecular microtubes, achieving structuring at multiple length scales and dimensionalities. The multistage self-assembly strategy involving hard co...

The internal structure of polyion assembly is usually ill-defined or less-ordered due to the inherent flexibility of polymers and nondirectionality of ionic interactions. Here we report polyion assemblies with well-defined, periodically regular internal structure on the basis of a stiff bisligand. We first build up a negatively charged supramolecul...

One of the recent challenges in nanotechnology is to construct ‘catalyzed self-assembly’. So far successful cases are still scarce. In this work we report a delicate case of cyclodextrin (α, β, γ-) CD catalyzed self-assembly of terthiophene-containing amphiphile TTC4L into microspheres. TT4CL may form amorphous precipitates without the assistance o...

The co-assembly of spherical colloids and surfactant-cyclodextrin microtubes yields a library of dynamic colloid-in-tube structures, including helices. In situ observations of these structures, including their thermo-reversible assembly and disassembly, demonstrate the potential of the interplay between molecular and colloidal self-assembly, thereb...

Hierarchische Selbstorganisation führt oft in der Natur zum Aufbau komplexer funktioneller Einheiten. Ein ähnlicher Ansatz, der die thermoreversible Coassemblierung sphärischer Kolloidpartikel und molekularer Mikroröhren nutzt, ergab dynamische Kolloid‐in‐Röhre‐Strukturen, wie kolloidale Zickzack‐Ketten, Doppel‐ und Tripelhelices. Der Auf‐ und Abba...

Hierarchical self-assembly is often exploited by nature to build complex functional entities. A similar approach yielded a library of dynamic colloid-in-tube structures, such as colloidal zigzags, double- and triple-helices, by utilizing the thermo-reversible co-assembly of colloidal spheres and molecular microtubes, as reported by J. Huang, A. V....

It is well known that the traditional tube theory of entangled polymer cannot provide a full picture of microscopic heterogeneity. However, problems on modern topics such as nanocomposites and cell motility require us to understand microscopic details of such systems. In order to study their dynamics, direct imaging of entangled biopolymer, F-actin...

Cross-linked networks are ubiquitous in synthetic and biological polymer systems, such as rubbers and cytoskeletons. To model cross-linked networks, several theories have been developed on the basis of different assumptions as to fluctuations in the networks. Here we put these theories to direct test. This talk will describe direct single-molecule...

We present here a host-guest approach to construct enzyme-triggered assembly systems on the basis of surfactant-cyclodextrin complexes and α-amylase. We realized enzyme-responsive model self-assembly systems including monolayers, micelles, and vesicles. The host-guest approach is expected to be extended to more complicated assembly systems with wid...

The properties and phase diagrams of aqueous mixtures of dodecyltrimethylammonium bromide (C(12)TAB) with the sodium oligoarene sulphonates (POSn), POS2, POS3, POS4, and POS6 have been studied using surface tension and neutron reflectometry to study the surface, and neutron small angle scattering and fluorescence to study the bulk solution. The beh...

Previously reported polymer-free cyclodextrin (CD) hydrogels usually relied on tailored modification of CDs or careful design and synthesis of guests, which may limit their mass production or application. Herein, we report on a hydrogel system based on a native CD (β-CD) and a commercially available zwitterionic surfactant (tetradecyl dimethylammon...

Recently, cyclodextrins (CDs) were found to play important yet complicated (or even apparently opposite sometimes) roles in self-assembly systems of amphiphiles or surfactants. Herein, we try to review and clarify the versatility of CDs in surfactant assembly systems by 1) classifying the roles played by CDs into two groups (modulator and building...

CDs may have promising functions in surfactant systems far beyond simply being disadvantageous to the formation of micelles. In this paper we review the recent literature and our work on the interesting effect of CDs on amphiphilic systems, especially on the concentrated single surfactant systems and catanionic surfactant mixed systems, both of the...

Cyclodextrin (CD)/surfactant complexes were usually believed to be quite soluble in water and unable to form aggregates because of the hydrophilic outer surface. However, in this work, SDS@2b-CD complex is found to be able to self-assemble into well-defined lamellar structures in concentrated aqueous solution. The lamellae possess unprecedented in-...

All salts studied effectively reduce critical micelle concentration (CMC) values of the cationic gemini surfactants. The ability to promote the surfactant aggregation decreases in the order of C(6)H(5)COONa > p-C(6)H(4)(COONa)(2) > Na(2)SO(4)> NaCl. Moreover, only C(6)H(5)COONa distinctly reduces both the CMC values and the surface tension at CMC....

We report in this work on the scaling behavior of wormlike micelles formed in a series of mixed systems of oppositely charged surfactants, including sodium decanote (SD)/hexadecyltrimethylammonium bromide (CTAB), sodium laurate (SL)/hexadecyltrimethylammonium bromide, sodium didecaminocystine (SDDC)/hexadecyltrimethylammonium bromide, and sodium di...

Traditional aqueous self-assembly of tubular structures (as well as other aggregates) usually relies on the hydrophobic effect, a relatively weak and nondirectional interaction. The resultant aggregates are inherently soft, fluid, and less-ordered. Alternatively, we report a novel kind of nonamphiphilic self-assembly of microtubes in aqueous soluti...

Cationic surfactant/anionic surfactant/beta-CD ternary aqueous systems provide a platform for the coexistence of the host-guest (beta-CD/surfactant) equilibrium and the biased aggregation (monomeric/aggregated surfactants) equilibrium. We report here that the interplay between the two equilibria dominates the systems as follows. (1) The biased aggr...

We report that the phase and self-assembly transition in an aqueous surfactant two-phase (ASTP) system can be induced by a small amount of glycerol. The ASTP was formed from a cationic Gemini surfactant, C12C6C12(Et), and an anionic surfactant, sodium laureate (SL), in a borax solution. Upon addition of 0.3-2 vol% glycerol to the system, the ASTP s...

Controllable aggregate transitions are achieved in this work by adding due amounts of beta-cyclodextrin (beta-CD) to mixed cationic/anionic surfactant aqueous solutions. In contrast to its "aggregate breaking" effect in single surfactant systems, aggregate growth is observed in nonstoichiometrical mixed cationic/anionic surfactant systems upon addi...

A noncovalent strategy is proposed for endowing responseless catanionic surfactant (a mixture of cationic and anionic surfactants) aggregates with responsive abilities by addition of a responser. In this strategy, the composition of catanionic surfactant can be carefully selected to render aggregates sensitive to added responsers, and the responser...

The vesicle-to-micelle transition (VMT) was realized in catanionic surfactant systems by the addition of two kinds of bile salts, sodium cholate (SC) and sodium deoxycholate (SDC). It was found that steric interaction between the bile salt and catanionic surfactant plays an important role in catanionic surfactant systems that are usually thought to...