"Life-like" nonequilibrium assemblies are of increasing significance, but suffering from limited steerability as they are generally based on micro/nanomotors with inherent asymmetry in chemical composition or geometry, of which the vigorous random Brownian rotations disturb the local interactions. Here, we demonstrate that isotropic photocatalytic micromotors, due to the persistent phoretic flow from the illuminated to shadowed side irrespective of their Brownian rotations, experience light-programmable local interactions (reversibly from attraction to repulsion and/or alignment) depending on the direction of the incident lights. Thus, they can be organized into a variety of tunable nonequilibrium assemblies, such as apolar solids (i.e., immobile colloidal crystal), polar liquids (i.e., phototactic colloidal stream), and polar solids (i.e., phototactic colloidal crystal), which can further be "cut" into a predesigned pattern by utilizing the switching motor-motor interactions at superimposed-light edges. This work facilitates the development of active matters and motile functional microdevices.
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http://dx.doi.org/10.34133/2022/9816562 | DOI Listing |
Polymers (Basel)
January 2025
Departamento de Química Física, Facultad de Ciencias Químicas, Universidad Complutense de Madrid, Ciudad Universitaria, Plaza de la Ciencias s/n, 28040 Madrid, Spain.
This study examines the adsorption and bulk assembly behaviour of quaternized hydroxyethylcellulose ethoxylate (QHECE)-sodium dodecyl sulphate (SDS) complexes on negatively charged substrates. Due to its quaternized structure, QHECE, which is used in several industries, including cosmetics, exhibits enhanced electrostatic interactions. The phase behaviour and adsorption mechanisms of QHECE-SDS complexes are investigated using model substrates that mimic the wettability and surface charge of damaged hair fibres.
View Article and Find Full Text PDFLangmuir
January 2025
Institute of Nano Science and Technology, Knowledge City, Sector 81, SAS Nagar, Mohali, Punjab 140306, India.
Enzyme-instructed signal generation at liquid-liquid interfaces presents a novel strategy for controlling and detecting biochemical processes on macroscopic scales. Here, we explore the self-assembly and jamming of pillar[5]arene (P[5]A) derivatives at the oil-water interface via a copper-mediated "click" reaction, providing a versatile platform for generating observable signals. The formation of a pillar[5]arenes network at the droplet interface reduces interfacial tension, allowing droplets to adopt various nonequilibrium shapes based on the interfacial jamming process.
View Article and Find Full Text PDFAcc Chem Res
January 2025
Department of Chemistry, Ben-Gurion University of the Negev, Be'er Sheva 84105, Israel.
ConspectusA key challenge in modern chemistry research is to mimic life-like functions using simple molecular networks and the integration of such networks into the first functional artificial cell. Central to this endeavor is the development of signaling elements that can regulate the cell function in time and space by producing entities of code with specific information to induce downstream activity. Such artificial signaling motifs can emerge in nonequilibrium systems, exhibiting complex dynamic behavior like bistability, multistability, oscillations, and chaos.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
Laboratoire Softmat, UMR au CNRS no 5623, Université Paul Sabatier, F-31062 Toulouse, France.
Simulations on an ODE-based model shows that there are many common points between Viedma deracemization and chiral self-assemblies of achiral building blocks towards chiral nanoparticles. Both systems occur in a closed system with energy exchange but no matter exchange with the surroundings and show parallel reversible growth mechanisms which coexist with an irreversible cluster breaking (grinding). The various mechanisms of growth give rise to the formation of polymerization/depolymerization cycles while the consecutive transformation of achiral monomer into chiral cluster results into an indirect enantioselective autocatalysis.
View Article and Find Full Text PDFACS Nano
January 2025
Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States.
With their ability to self-assemble spontaneously into well-defined nanoscale morphologies, block copolymer (BCP) thin films are a versatile platform to fabricate functional nanomaterials. An important challenge to wider deployment of BCPs in nanofabrication is combining precise control over the nanoscale domain orientation in BCP assemblies with scalable deposition techniques that are applicable to large-area, curved, and flexible substrates. Here, we show that spray-deposited smooth films of a nominally disordered BCP exhibit latent orientations, which can be prescriptively selected by controlling solvent evaporation during spray casting.
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