Growth Mediated Disassembly of Cucurbit[8]uril Cross‐linked Static Cubic Self‐assembly of Silver Nanoparticles DOI
Sancharika Dalal, Kalyan K. Sadhu

ChemNanoMat, Journal Year: 2024, Volume and Issue: unknown

Published: July 23, 2024

Abstract Static self‐assembly resides in thermodynamically stable global minima of the energy landscape, whereas dynamic occupies local profile and remains ordered state for a limited time via dissipation to surroundings. This makes spatiotemporal control over assembly disassembly mechanism easily controllable case self‐assembly. However, due higher thermal stability static self‐assembly, it is very challenging perform reverse engineering on these types systems. Herein we report growth reaction‐based reversal silver cubes obtained cucurbit[8]uril (CB[8]) crosslinked nanoparticles (AgNP). The AgNP building units with variable CB[8] surface coverage have been used as seeds onto which deposition gold reaction has performed. supracube structure controlled by formation [AuCl 4 ] − –CB[8] complex successive reduction Au 0 seed. resulting monodispersed isotropic nanoparticles, formed from based cubic after growth, exhibit Au−Ag bimetallic nature. Quenching fluorogenic response hydrophobic dye coumarin‐7, added suggests direct interaction metallic nanoparticle thereby confirms successful mediated

Language: Английский

Observing the Dynamics of an Electrochemically Driven Active Material with Liquid Electron Microscopy DOI
Wyeth Gibson, Justin T. Mulvey, Swetamber Das

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(18), P. 11898 - 11909

Published: April 22, 2024

Electrochemical liquid electron microscopy has revolutionized our understanding of nanomaterial dynamics by allowing for direct observation their electrochemical production. This technique, primarily applied to inorganic materials, is now being used explore the self-assembly active molecular materials. Our study examines these across various scales, from nanoscale behavior individual fibers micrometer-scale hierarchical evolution fiber clusters. To isolate influences beam and electrical potential on material behavior, we conducted thorough beam–sample interaction analyses. findings reveal that materials at are shaped proximity electrode current. By integrating observations with reaction–diffusion simulations, uncover local structures formation history play a crucial role in determining assembly rates. suggests emergence nonequilibrium can locally accelerate further structural development, offering insights into under conditions.

Language: Английский

Citations

4
Transient colloidal crystals fueled by electrochemical reaction products DOI Creative Commons

Medha Rath,

Satyam Srivastava, Eric A. Carmona

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Feb. 28, 2025

Conventional electric field directed colloidal assembly enables fabricating ordered structures but lacks temporal control over state. Chemical reaction networks have been discovered that transiently assemble colloids; however, they slow dynamics (hrs – days) and poor tunability, utilize complex reagents, produce kinetically trapped states. Here we demonstrate transient crystals autonomously form, breakup, reconstitute in response to an electrochemical network driven by a time invariant electrical stimulus. Aqueous mixtures of micron sized colloids para-benzoquinone (BQ) were subjected superimposed oscillatory steady potentials, i.e., multimode induce electrokinetic flows around proton-coupled BQ redox reactions. Transient states coincided with electrochemically generated pH spikes near the cathode. We wide tunability state lifetimes two orders magnitude modifying potential electrode separation. An transport model showed interaction advancing acidic alkaline fronts from anodic oxidation cathodic reduction caused transients. present theoretical experimental evidence indicates mediated competition between opposing scale electrohydrodynamic electroosmotic flows, latter which is dependent. methods for struggle This study demonstrates disassemble, reassemble network, achieving using potentials.

Language: Английский

Citations

0
Dissipation rates from experimental uncertainty DOI Creative Commons
Aishani Ghosal, Jason R. Green

Physical Review Research, Journal Year: 2025, Volume and Issue: 7(1)

Published: March 24, 2025

Active matter and driven systems exhibit statistical fluctuations in density particle positions that are an indirect indicator of dissipation across length time scales. Here, we quantitatively relate these to a thermodynamic speed limit constrains the rates heat entropy production nonequilibrium processes. By reparametrizing set by Fisher information, show how infer from directly observable or controllable quantities. This approach can use available experimental data as input avoid need for analytically solvable microscopic models full time-dependent probability distributions. The rate predict agrees with measurements pulled Brownian microtubule active gel, which validates suggests potential design experiments. Published American Physical Society 2025

Language: Английский

Citations

0
Chemically-Fueled Phase Transition of a redox-responsive polymer DOI Creative Commons
Takafumi Enomoto, Aya Mizutani Akimoto, Ryo Yoshida

et al.

Science and Technology of Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 22, 2025

Language: Английский

Citations

0
Time‐Encoded Information Encryption with pH Clock Guided Broad‐Spectrum Emission by Dynamic Assemblies DOI
Debapratim Das,

Priyam Das,

Tanushree Das

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 22, 2024

With growing threats from counterfeiting-based security breaches, multi-level and specific stimuli-responsive anti-counterfeiting devices message encryption methods have attracted immense research interest. Fluorescence-based aggregation-induced emission (AIE)-based materials solves the problems to a considerable extent. However, development of smarter patterns with hierarchical levels alongside dynamic display is still challenging. To screen out this complication, we bring forward pH-switchable fluorescent assembly an AIEgen aliphatic acid. We later temporally direct molecular aid chemical trigger-regulated pH clock, generating transitory multicolor emission, including transient white light generation. The pH-dependent emissions were further implemented in constructing smart multi-input AND gates. Subsequently, integrate time-gated emissive system develop advanced multi-dimensionally secure data strategy. This novel approach enhances measures by introducing additional layer based on temporal characteristics.

Language: Английский

Citations

2
Time‐Encoded Information Encryption with pH Clock Guided Broad‐Spectrum Emission by Dynamic Assemblies DOI
Debapratim Das,

Priyam Das,

Tanushree Das

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 22, 2024

Abstract With growing threats from counterfeiting‐based security breaches, multi‐level and specific stimuli‐responsive anti‐counterfeiting devices message encryption methods have attracted immense research interest. Fluorescence‐based aggregation‐induced emission (AIE)‐based materials solves the problems to a considerable extent. However, development of smarter patterns with hierarchical levels alongside dynamic display is still challenging. To screen out this complication, we bring forward pH‐switchable fluorescent assembly an AIEgen aliphatic acid. We later temporally direct molecular aid chemical trigger‐regulated pH clock, generating transitory multicolor emission, including transient white light generation. The pH‐dependent emissions were further implemented in constructing smart multi‐input AND gates. Subsequently, integrate time‐gated emissive system develop advanced multi‐dimensionally secure data strategy. This novel approach enhances measures by introducing additional layer based on temporal characteristics.

Language: Английский

Citations

2
Cell‐Like Synthetic Supramolecular Soft Materials Realized in Multicomponent, Non‐/Out‐of‐Equilibrium Dynamic Systems DOI Creative Commons
Ryou Kubota, Itaru Hamachi

Advanced Science, Journal Year: 2023, Volume and Issue: 11(8)

Published: Nov. 28, 2023

Abstract Living cells are complex, nonequilibrium supramolecular systems capable of independently and/or cooperatively integrating multiple bio‐supramolecules to execute intricate physiological functions that cannot be accomplished by individual biomolecules. These biological design strategies offer valuable insights for the development synthetic with spatially controlled hierarchical structures, which, importantly, exhibit cell‐like responses and functions. The next grand challenge in chemistry is control organization types supramolecules a single system, thus these an orthogonal cooperative manner. In this perspective, recent progress constructing multicomponent soft materials through hybridization supramolecules, such as self‐assembled nanofibers/gels coacervates, other functional molecules, including polymer gels enzymes highlighted. Moreover, results show bioinspired stimuli, bidirectional rheological double‐network hydrogels, temporal stimulus pattern‐dependent 3D hydrogel patterning response reaction–diffusion processes presented. Autonomous active structures hold promise diverse applications, robotics directional motion, point‐of‐care disease diagnosis, tissue regeneration.

Language: Английский

Citations

6
Transient and directional growth of supramolecular hydrogels through reaction–diffusion-mediated self-assembly for dynamic wet gluing DOI

Shengyu Bai,

Hucheng Wang,

Guanyao Gu

et al.

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 475, P. 146125 - 146125

Published: Sept. 18, 2023

Language: Английский

Citations

6
CryoEM reveals the complex self-assembly of a chemically driven disulfide hydrogel DOI Creative Commons
Paul J. Hurst, Justin T. Mulvey, Rebecca A. Bone

et al.

Chemical Science, Journal Year: 2023, Volume and Issue: 15(3), P. 1106 - 1116

Published: Dec. 18, 2023

We elucidate the mechanisms of chemically driven self-assembly processes, demonstrating how synchronous assembly–disassembly reactions can stabilize transient structures and create morphologies that differ from conventional assemblies.

Language: Английский

Citations

4
Emergence of Dynamic Instability by Hybridizing Synthetic Self-Assembled Dipeptide Fibers with Surfactant Micelles DOI

Shogo Torigoe,

Kazutoshi Nagao,

Ryou Kubota

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(9), P. 5799 - 5805

Published: Feb. 26, 2024

Supramolecular chemistry currently faces the challenge of controlling nonequilibrium dynamics such as dynamic instability microtubules. In this study, we explored emergence through hybridization peptide-type supramolecular nanofibers with surfactant micelles. Using real-time confocal imaging, discovered that addition micelles to induced simultaneous but asynchronous growth and shrinkage during which total number fibers decreased monotonically. This phenomenon unexpectedly persisted for 6 days was driven not by chemical reactions noncovalent interactions between study demonstrates a strategy inducing autonomous dynamics, will open up possibilities developing soft materials applicable biomedicine robotics.

Language: Английский

Citations

1