Wavelength-Selective Light-Responsive DASA-Functionalized Polymersome Nanoreactors DOI
Omar Rifaie‐Graham, Sebastian Ulrich, Nikolas F. B. Galensowske

et al.

Journal of the American Chemical Society, Journal Year: 2018, Volume and Issue: 140(25), P. 8027 - 8036

Published: June 1, 2018

Transient activation of biochemical reactions by visible light and subsequent return to the inactive state in absence is an essential feature processes photoreceptor cells. To mimic such light-responsiveness with artificial nanosystems, polymersome nanoreactors were developed that can be switched on self-revert fast dark at room temperature their state. Donor–acceptor Stenhouse adducts (DASAs), ability isomerize upon irradiation light, employed change permeability membranes switching polarity from a nonpolar triene-enol form cyclopentenone increased polarity. this end, amphiphilic block copolymers containing poly(pentafluorophenyl methacrylate) hydrophobic synthesized reversible addition–fragmentation chain-transfer (RAFT) radical polymerization functionalized either DASA based Meldrum’s acid or novel fast-switching pyrazolone-based DASA. These polymers self-assembled into vesicles. Release hydrophilic payload could triggered stopped as soon was turned off. The encapsulation enzymes yielded photoresponsive catalyzed only if they irradiated light. A mixture nanoreactors, one switches green other red permitted specific control individual reaction cascade pot varied wavelengths, thus enabling light-controlled wavelength-selective catalysis. DASA-based demonstrate potential DASAs switch find application off, demand, e.g., microfluidics drug delivery.

Language: Английский

Photochromism into nanosystems: towards lighting up the future nanoworld DOI
Ling Wang, Quan Li

Chemical Society Reviews, Journal Year: 2017, Volume and Issue: 47(3), P. 1044 - 1097

Published: Dec. 18, 2017

This review provides a state-of-the-art account of photochromism into diverse functional nanosystems such as nanomachines, nanoparticles, nanoelectronics, nanoassemblies and biological nanosystems.

Language: Английский

Citations

664

Photo- and Redox-Driven Artificial Molecular Motors DOI Creative Commons
Massimo Baroncini, Serena Silvi, Alberto Credi

et al.

Chemical Reviews, Journal Year: 2019, Volume and Issue: 120(1), P. 200 - 268

Published: Aug. 15, 2019

Directed motion at the nanoscale is a central attribute of life, and chemically driven motor proteins are nature’s choice to accomplish it. Motivated inspired by such bionanodevices, in past few decades chemists have developed artificial prototypes molecular motors, namely, multicomponent synthetic species that exhibit directionally controlled, stimuli-induced movements their parts. In this context, photonic redox stimuli represent highly appealing modes activation, particularly from technological viewpoint. Here we describe evolution field photo- redox-driven provide comprehensive review work published 5 years. After an analysis general principles govern controlled directed movement scale, fundamental photochemical processes can enable its realization. The main classes light- motors illustrated, with particular focus on recent designs, thorough description functions performed these kinds devices according literature reports presented. Limitations, challenges, future perspectives critically discussed.

Language: Английский

Citations

454

Enlightening Materials with Photoswitches DOI Creative Commons
Alexis Goulet‐Hanssens, Fabian Eisenreich, Stefan Hecht

et al.

Advanced Materials, Journal Year: 2020, Volume and Issue: 32(20)

Published: Jan. 24, 2020

Incorporating molecular photoswitches into various materials provides unique opportunities for controlling their properties and functions with high spatiotemporal resolution using remote optical stimuli. The great largely still untapped potential of these photoresponsive systems has not yet been fully exploited due to the fundamental challenges in harnessing geometrical electronic changes on level modulate macroscopic bulk material properties. Herein, progress made during past decade field photoswitchable is highlighted. After pointing some general design principles, an increasing order integrated units are discussed, spanning range from amorphous settings over surfaces/interfaces supramolecular ensembles, liquid crystalline phases. Finally, future directions pointed out conclusion. In view exciting recent achievements field, emergence further development light-driven optically programmable (inter)active eagerly anticipated.

Language: Английский

Citations

436

Energy consumption in chemical fuel-driven self-assembly DOI
Giulio Ragazzon, Leonard J. Prins

Nature Nanotechnology, Journal Year: 2018, Volume and Issue: 13(10), P. 882 - 889

Published: Sept. 11, 2018

Language: Английский

Citations

415

Advances in theE → ZIsomerization of Alkenes Using Small Molecule Photocatalysts DOI
Tomáš Neveselý,

Max Wienhold,

John J. Molloy

et al.

Chemical Reviews, Journal Year: 2021, Volume and Issue: 122(2), P. 2650 - 2694

Published: Aug. 27, 2021

Geometrical E → Z alkene isomerization is intimately entwined in the historical fabric of organic photochemistry and enjoying a renaissance (Roth et al. Angew. Chem., Int. Ed. Engl. 1989 28, 1193–1207). This consequence fundamental stereochemical importance Z-alkenes, juxtaposed with frustrations thermal reactivity that are rooted microscopic reversibility. Accessing excited state paradigms allow this latter obstacle to be circumnavigated by exploiting subtle differences photophysical behavior substrate product chromophores: provides molecular basis for directionality. While direct irradiation operationally simple, photosensitization via selective energy transfer enables augmentation repertoire include substrates not directly photons. Through sustained innovation, an impressive portfolio tailored small molecule catalysts range triplet energies now widely available facilitate contra-thermodynamic thermo-neutral reactions generate Z-alkene fragments. review intended serve as practical guide covering geometric alkenes enabled catalysis from 2000 2020, logical sequel excellent treatment Dugave Demange (Chem. Rev. 2003 103, 2475–2532). The mechanistic foundations underpinning selectivity discussed together induction models rationales explain counterintuitive directionality these processes which very distinguish product. Implications subsequent stereospecific transformations, application total synthesis, regioselective polyene isomerization, spatiotemporal control pre-existing configuration broader sense discussed.

Language: Английский

Citations

309

Viewpoint: From Responsive to Adaptive and Interactive Materials and Materials Systems: A Roadmap DOI Creative Commons
Andreas Walther

Advanced Materials, Journal Year: 2019, Volume and Issue: 32(20)

Published: Nov. 25, 2019

Soft matter systems and materials are moving toward adaptive interactive behavior, which holds outstanding promise to make the next generation of intelligent soft inspired from dynamics behavior living systems. But what is an material? What How should classical responsiveness or smart be delineated? At present, literature lacks a comprehensive discussion on these topics, however profound importance in order identify landmark advances, keep correct noninflating terminology, most importantly educate young scientists going into this direction. By comparing different levels complex biological systems, Viewpoint strives give some definition various characteristics. In particular, thinking direction training learning materials, metabolic behavioral highlighted, as well communication information-processing This aims also serve switchboard further connect important fields chemistry, synthetic biology, supramolecular chemistry nano- microfabrication/3D printing with advanced research. A convergence disciplines will at heart empowering future increasingly emergent life-like behavior.

Language: Английский

Citations

264

Chemically Fueled Self‐Assembly in Biology and Chemistry DOI Creative Commons
Krishnendu Das, Luca Gabrielli, Leonard J. Prins

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(37), P. 20120 - 20143

Published: March 11, 2021

Life is a non-equilibrium state of matter maintained at the expense energy. Nature uses predominantly chemical energy stored in thermodynamically activated, but kinetically stable, molecules. These high-energy molecules are exploited for synthesis other biomolecules, activation biological machinery such as pumps and motors, maintenance structural order. Knowledge how transferred to biochemical processes essential development artificial systems with life-like processes. Here, we discuss can be used control organization organic Four different strategies have been identified according distinguishable physical-organic basis. For each class, one example from biology chemistry discussed detail illustrate practical implementation concept distinct opportunities they offer. Specific attention paid discussion chemically fueled self-assembly. We meaning self-assembly, its kinetic origin, develop synthetic systems.

Language: Английский

Citations

259

Light - driven deracemization enabled by excited - state electron transfer DOI Open Access
Nick Shin, Jonathan M. Ryss, Xin Zhang

et al.

Science, Journal Year: 2019, Volume and Issue: 366(6463), P. 364 - 369

Published: Oct. 17, 2019

Charging through the looking glass Asymmetric catalysis is a commonly applied technique to prepare just one of two mirror-image products in chemical reaction. But what if you already have compound want, stuck mixture left- and right-handed enantiomers? Shin et al. now show that light-induced electron transfer can trigger favorable succession proton hydrogen-atom steps, both which are susceptible biasing by catalysts, preferentially convert cyclic urea enantiomers into (see Perspective Wendlandt). Science , this issue p. 364 ; see also 304

Language: Английский

Citations

230

A Redox Strategy for Light-Driven, Out-of-Equilibrium Isomerizations and Application to Catalytic C–C Bond Cleavage Reactions DOI
Eisuke Ota, Huaiju Wang,

Nils Lennart Frye

et al.

Journal of the American Chemical Society, Journal Year: 2019, Volume and Issue: 141(4), P. 1457 - 1462

Published: Jan. 10, 2019

We report a general protocol for the light-driven isomerization of cyclic aliphatic alcohols to linear carbonyl compounds. These reactions proceed via proton-coupled electron-transfer activation alcohol O–H bonds followed by subsequent C–C β-scission resulting alkoxy radical intermediates. In many cases, these redox-neutral isomerizations in opposition significant energetic gradient, yielding products that are less thermodynamically stable than starting materials. A mechanism is presented rationalize this out-of-equilibrium behavior may serve as model design other contrathermodynamic transformations driven excited-state redox events.

Language: Английский

Citations

207

New molecular switch architectures DOI Open Access
Jared D. Harris,

Mark Moran,

Ivan Aprahamian

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2018, Volume and Issue: 115(38), P. 9414 - 9422

Published: July 16, 2018

In this paper we elaborate on recently developed molecular switch architectures and how these new systems can help with the realization of functions advancement artificial machines. Progress in chemically photoinduced switches motors is summarized contextualized such that reader may gain an appreciation for novel tools have come about past decade. Many offer distinct advantages over commonly employed switches, including improved fidelity, addressability, robustness. Thus, serves as a jumping-off point researchers seeking switching motifs specific applications, or ones address limitations presently available systems.

Language: Английский

Citations

203