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

и другие.

Journal of the American Chemical Society, Год журнала: 2018, Номер 140(25), С. 8027 - 8036

Опубликована: Июнь 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.

Язык: Английский

Boron-enabled geometric isomerization of alkenes via selective energy-transfer catalysis DOI
John J. Molloy,

Michael Schäfer,

Max Wienhold

и другие.

Science, Год журнала: 2020, Номер 369(6501), С. 302 - 306

Опубликована: Июль 17, 2020

An E-Z boron swivel Compounds with carbon-carbon double bonds can form two distinct isomers, depending on whether the heaviest substituents both carbons lie same side (labeled Z) or diagonally across from each other E). Molloy et al. present a convenient method to reorient that bear and carbonyl substituents. When they are opposed, stay in plane, bond is easily swiveled by photosensitization. However, once as carbonyl, rotates out of plane further sensitization inhibited. Science this issue p. 302

Язык: Английский

Процитировано

186

Dissipative Self-Assembly: Fueling with Chemicals versus Light DOI Creative Commons
Maren Weißenfels, Julius Gemen,

Rafał Klajn

и другие.

Chem, Год журнала: 2021, Номер 7(1), С. 23 - 37

Опубликована: Янв. 1, 2021

Язык: Английский

Процитировано

173

Targeting drug delivery with light: A highly focused approach DOI Creative Commons
Teresa L. Rapp, Cole A. DeForest

Advanced Drug Delivery Reviews, Год журнала: 2021, Номер 171, С. 94 - 107

Опубликована: Янв. 22, 2021

Язык: Английский

Процитировано

129

Multi-stimuli Control over Assembly and Guest Binding in Metallo-supramolecular Hosts Based on Dithienylethene Photoswitches DOI Creative Commons

Ru‐Jin Li,

Jacopo Tessarolo, Haeri Lee

и другие.

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(10), С. 3865 - 3873

Опубликована: Март 5, 2021

It is difficult to assemble multi-component metallo-supramolecular architectures in a non-statistical fashion, which limits their development toward functional materials. Herein, we report system of interconverting bowls and cages that are able respond various selective stimuli (light, ligands, anions), based on the self-assembly photochromic dithienylethene (DTE) ligand, La, with PdII cations. By combining concept "coordination sphere engineering", relying bulky quinoline donors, reversible photoswitching between ligand's open (o-La) closed (c-La) forms, [Pd2(o-La)4] cage (o-C) [Pd2(c-La)3] bowl (c-B) were obtained, respectively. This structural rearrangement modulates system's guest uptake capabilities. Among three bis-sulfonate guests (G1, G2, G3), can encapsulate only smallest (G1), while binds all them. Bowl c-B was further used synthesize series heteroleptic cages, [Pd2LA3LB], representing motif never reported before. Additional ligands (Lc-f), short or long arms, tune cavity size, thus enabling preventing uptake. Addition Br-/Ag+ makes it possible change overall charge, again triggering release, as well fourth ligand de-/recomplexation. In combination, site-selective introduction functionality application external lead an intricate hosts different preferences. A high degree complexity achieved through cooperativity few components.

Язык: Английский

Процитировано

125

Dynamics of Excitons in Conjugated Molecules and Organic Semiconductor Systems DOI
Oleg P. Dimitriev

Chemical Reviews, Год журнала: 2022, Номер 122(9), С. 8487 - 8593

Опубликована: Март 17, 2022

The exciton, an excited electron-hole pair bound by Coulomb attraction, plays a key role in photophysics of organic molecules and drives practically important phenomena such as photoinduced mechanical motions molecule, photochemical conversions, energy transfer, generation free charge carriers, etc. Its behavior extended π-conjugated disordered films is very different rich compared with exciton inorganic semiconductor crystals. Due to the high degree variability systems themselves, not only exerts changes on that carry it but undergoes its own during all phases lifetime, is, birth, conversion transport, decay. goal this review give systematic comprehensive view molecular assemblies at evolution emphasis rates typical for dynamic picture various consequences above dynamics. To uncover variety behavior, details formation, conversion, direct reverse intersystem crossing, radiative nonradiative decay are considered systems, where these processes lead or influenced static disorder, distribution symmetry breaking, reactions, electron proton structural rearrangements, coupling vibrations intermediate particles, dissociation annihilation well.

Язык: Английский

Процитировано

124

Chemical engines: driving systems away from equilibrium through catalyst reaction cycles DOI
Shuntaro Amano, Stefan Borsley, David A. Leigh

и другие.

Nature Nanotechnology, Год журнала: 2021, Номер 16(10), С. 1057 - 1067

Опубликована: Окт. 1, 2021

Язык: Английский

Процитировано

108

A Highly Dynamic Covalent Polymer Network without Creep: Mission Impossible? DOI
Filip Van Lijsebetten, Tapas Debsharma, Johan M. Winne

и другие.

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(48)

Опубликована: Сен. 26, 2022

Dynamic covalent polymer networks provide an interesting solution to the challenging recyclability of thermosets and elastomers. One remaining design constraints, however, is balancing thermal reprocessability in form material flow with dimensional stability during use. As a result, many chemistries are being investigated order improve bond reactivity control robustness. This Minireview highlights number promising concepts, particular emphasis on disconnecting chemical low high temperature regimes obtain creep resistant, yet highly dynamic networks. In addition, we will highlight impact sharp changes when applying extrapolation-based approaches rheological analysis. confident that abandoning myth "permanent" aid development sustainable polymeric materials can truly combine benefits thermoplastic thermoset behaviour.

Язык: Английский

Процитировано

98

A Dihydroazulene‐Based Photofluorochromic AIE System for Rewritable 4D Information Encryption DOI
Jianyu Zhang, Hanchen Shen,

Xinyue Liu

и другие.

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(37)

Опубликована: Июль 16, 2022

Dynamic patterns based on luminescent materials play an essential role in the digital age. However, it is still challenging to develop highly emissive photofluorochromic with dynamic behaviors store information multiple characteristics. Here, we report a series of dihydroazulene-based compounds which show typical aggregation-induced emission (AIE) effect. Moreover, photo-switching ability dihydroazulene units, undergoing light-induced ring-opening, enables properties. The photofluorochromism also shows quantitively described responses time and temperature via reverse ring-closing process. Ultimately, rewritable 4D system, embedded quick response code, dot matrix microstructures, color fluorescence, time/temperature-dependent intensity change, established patterns. This work not only develops AIE skeleton properties but provides new strategy for encryption cybernetics.

Язык: Английский

Процитировано

78

Kinetic and energetic insights into the dissipative non-equilibrium operation of an autonomous light-powered supramolecular pump DOI
Stefano Corrà, Marina Tranfić Bakić, Jessica Groppi

и другие.

Nature Nanotechnology, Год журнала: 2022, Номер 17(7), С. 746 - 751

Опубликована: Июнь 27, 2022

Язык: Английский

Процитировано

73

Nanoparticle Self-Assembly: From Design Principles to Complex Matter to Functional Materials DOI
Anish Rao, Sumit Roy, Vanshika Jain

и другие.

ACS Applied Materials & Interfaces, Год журнала: 2022, Номер 15(21), С. 25248 - 25274

Опубликована: Июнь 17, 2022

The creation of matter with varying degrees complexities and desired functions is one the ultimate targets self-assembly. ability to regulate complex interactions between individual components essential in achieving this target. In direction, initial success controlling pathways final thermodynamic states a self-assembly process promising. Despite progress made field, there has been growing interest pushing limits processes. main inception that intended self-assembled state, complexities, may not be "at equilibrium (or at global minimum)", rendering free energy minimization unsuitable form product. Thus, we believe thorough understanding design principles as well predict outcome collection next generation matter. present review highlights potent role finely tuned interparticle nanomaterials achieve preferred structures properties. We bringing prediction nanoparticle processes will have similar effect retrosynthesis had on logic chemical synthesis. Along guiding principles, gives summary different types products created from assemblies functional properties emerging them. Finally, highlight reasonable expectations field challenges lying ahead evolvable

Язык: Английский

Процитировано

72