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1.
Nature ; 597(7878): 655-659, 2021 09.
Artigo em Inglês | MEDLINE | ID: mdl-34588672

RESUMO

In 1878, Lord Rayleigh observed the highly celebrated phenomenon of sound waves that creep around the curved gallery of St Paul's Cathedral in London1,2. These whispering-gallery waves scatter efficiently with little diffraction around an enclosure and have since found applications in ultrasonic fatigue and crack testing, and in the optical sensing of nanoparticles or molecules using silica microscale toroids. Recently, intense research efforts have focused on exploring non-Hermitian systems with cleverly matched gain and loss, facilitating unidirectional invisibility and exotic characteristics of exceptional points3,4. Likewise, the surge in physics using topological insulators comprising non-trivial symmetry-protected phases has laid the groundwork in reshaping highly unconventional avenues for robust and reflection-free guiding and steering of both sound and light5,6. Here we construct a topological gallery insulator using sonic crystals made of thermoplastic rods that are decorated with carbon nanotube films, which act as a sonic gain medium by virtue of electro-thermoacoustic coupling. By engineering specific non-Hermiticity textures to the activated rods, we are able to break the chiral symmetry of the whispering-gallery modes, which enables the out-coupling of topological 'audio lasing' modes with the desired handedness. We foresee that these findings will stimulate progress in non-destructive testing and acoustic sensing.

2.
Phys Rev Lett ; 131(6): 066601, 2023 Aug 11.
Artigo em Inglês | MEDLINE | ID: mdl-37625050

RESUMO

The Su-Schrieffer-Heeger (SSH) model is an important cornerstone in modern condensed-matter topology, yet it is the simplest one-dimensional (1D) tight binding approach to dwell into the characteristics of spinless electrons in chains of staggered bonds. Moreover, the chiral symmetry assures that its surface-confining states pin to zero energy, i.e., they reside midgap in the energy dispersion. Symmetry is also an attribute related to artificial media that are subject to parity P and time-reversal T operations. This non-Hermitian family has been thoroughly nourished in a wave-based context, where anti-PT (APT) symmetric systems are the youngest belonging members, permitting refractionless optics, inverse PT-symmetry breaking transition, and asymmetric mode switching. Here, we report the first extension of APT symmetry in an acoustic setting by endowing a SSH lattice with gain and loss components. We show that the in-gap topological defect state hinges on the non-Hermitian phase, in that the broken symmetry suppresses it, yet when PT or APT symmetry is intact, it is observed with either damped or evanescent decay, respectively. Our experiments showcase how the non-Hermitian SSH lattice serves as a utile platform to investigate topological properties across various PT symmetric phases using sound.

3.
Org Biomol Chem ; 16(10): 1736-1744, 2018 03 07.
Artigo em Inglês | MEDLINE | ID: mdl-29459926

RESUMO

A straightforward method for the synthesis of polyfunctionalized quinolines from readily available N-aryl propargylamines under aerobic conditions was developed. It provides convenient access to a variety of synthetically and pharmaceutically important quinolines in moderate to good yields. Control experiments suggest that the cascade reaction might proceed via the Pd-catalyzed electrophilic cyclization of N-aryl propargylamines followed by a hydroarylation process through trapping of the σ-quinolinylpalladium intermediate with a second molecule of the substrate.

4.
J Org Chem ; 82(20): 11247-11252, 2017 10 20.
Artigo em Inglês | MEDLINE | ID: mdl-28957630

RESUMO

A new one-pot strategy for the synthesis of quinoxalin-2-ones from the tandem nitrosation/cyclization reaction of N-aryl cyanoacetamides with tert-butyl nitrite has been developed. The dehydrogenative N-incorporation is achieved through a sequence of nitrosation, tautomerization, and cyclization, affording quinoxalin-2-ones in moderate to good yields with good functional group tolerance.

5.
J Org Chem ; 81(18): 8647-52, 2016 09 16.
Artigo em Inglês | MEDLINE | ID: mdl-27560461

RESUMO

A copper-catalyzed three-component tandem reaction has been developed for the convenient and practical synthesis of 1,4-benzothiazines. A variety of terminal alkynes and 2-iodo/bromophenyl isothiocyanates underwent this one-pot cyclization with aqueous ammonia to afford 1,4-benzothiazines in moderate to good yields.

6.
J Org Chem ; 81(13): 5710-6, 2016 07 01.
Artigo em Inglês | MEDLINE | ID: mdl-27232156

RESUMO

A tandem annulation of arylpropynols with disulfides has been developed for the synthesis of 2-sulfenylindenone derivatives. The reaction pathway involves one-pot tandem Meyer-Schuster rearrangement of arylpropynols and successive radical cyclization with disulfides. Various arylpropynols and disulfides with a number of functional groups are compatible in this reaction that affords the corresponding 2-sulfenylindenones in moderate to good yields.

7.
Org Biomol Chem ; 13(10): 3122-7, 2015 Mar 14.
Artigo em Inglês | MEDLINE | ID: mdl-25632941

RESUMO

A new ring expansion of 2-aminobenzothiazoles with alkynyl carboxylic acids was developed, which allows for one-pot synthesis of 1,4-benzothiazines in moderate to excellent yields. The cascade reaction was achieved through decarboxylative coupling, nucleophilic ring-opening reaction and intramolecular hydroamination process.


Assuntos
Ácidos Carboxílicos/química , Cobre/química , Tiazinas/síntese química , Tiazóis/química , Catálise , Espectroscopia de Ressonância Magnética , Estrutura Molecular , Solventes/química , Temperatura
8.
J Org Chem ; 79(20): 9907-12, 2014 Oct 17.
Artigo em Inglês | MEDLINE | ID: mdl-25244055

RESUMO

An iron-promoted tandem carboxamidation and cyclization between aryl isonitriles and formamides has been developed. The one-pot strategy can be applied to a wide range of 2-isocyanobiphenyls and formamides with excellent functional group tolerance for the synthesis of phenanthridine-6-carboxamides in moderate to excellent yields.


Assuntos
Cloretos/química , Compostos Férricos/química , Formamidas/química , Nitrilas/química , Fenantridinas/química , Fenantridinas/síntese química , Catálise , Ciclização , Estrutura Molecular , Estereoisomerismo
9.
J Org Chem ; 78(3): 1300-5, 2013 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-23305155

RESUMO

A palladium-catalyzed, iodine-mediated electrophilic annulation between 2-(1-alkynyl)biphenyl and disulfide has been developed. With the combination of PdCl(2) and I(2), a variety of 2-(1-alkynyl)biphenyls underwent electrophilic annulations with various disulfides successfully to afford the corresponding 9-sulfenyl phenanthrenes in moderate to excellent yields.


Assuntos
Alcinos/química , Compostos de Bifenilo/química , Dissulfetos/química , Iodo/química , Paládio/química , Catálise , Estrutura Molecular
10.
J Org Chem ; 78(12): 6025-30, 2013 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-23710680

RESUMO

A palladium-catalyzed tandem Suzuki/C-H arylation reaction of N-aryltrifluoroacetimidoyl chlorides with arylboronic acids has been developed. A variety of 6-(trifluoromethyl)phenanthridines were prepared in moderate to excellent yields from N-(2-bromophenyl)trifluoroacetimidoyl chlorides which can be conveniently prepared from 2-bromoaniline derivatives.


Assuntos
Paládio/química , Fenantridinas/síntese química , Compostos de Anilina/química , Ácidos Borônicos/química , Catálise , Estrutura Molecular
11.
Int J Mol Sci ; 13(11): 15162-76, 2012 Nov 16.
Artigo em Inglês | MEDLINE | ID: mdl-23203117

RESUMO

Proteinase inhibitors play an important role in plant resistance of insects and pathogens. In this study, we characterized the serine proteinase inhibitor SaPIN2b, which is constitutively expressed in Solanum americanum trichomes and contains two conserved motifs of the proteinase inhibitor II (PIN2) family. The recombinant SaPIN2b (rSaPIN2b), which was expressed in Escherichia coli, was demonstrated to be a potent proteinase inhibitor against a panel of serine proteinases, including subtilisin A, chymotrypsin and trypsin. Moreover, rSaPIN2b also effectively inhibited the proteinase activities of midgut trypsin-like proteinases that were extracted from the devastating pest Helicoverpa armigera. Furthermore, the overexpression of SaPIN2b in transgenic tobacco plants resulted in enhanced resistance against H. armigera. Taken together, our results demonstrated that SaPIN2b is a potent serine proteinase inhibitor that may act as a protective protein in plant defense against insect attacks.


Assuntos
Proteínas de Plantas/farmacologia , Inibidores de Serina Proteinase/farmacologia , Solanum/química , Tricomas/química , Sequência de Aminoácidos , Animais , Relação Dose-Resposta a Droga , Expressão Gênica , Dados de Sequência Molecular , Mariposas/enzimologia , Proteínas de Plantas/química , Proteínas de Plantas/genética , Proteínas de Plantas/isolamento & purificação , Plantas Geneticamente Modificadas , Proteínas Recombinantes/química , Proteínas Recombinantes/genética , Proteínas Recombinantes/isolamento & purificação , Proteínas Recombinantes/farmacologia , Alinhamento de Sequência , Inibidores de Serina Proteinase/química , Inibidores de Serina Proteinase/isolamento & purificação , Nicotiana/genética , Nicotiana/parasitologia
12.
Org Lett ; 24(29): 5386-5390, 2022 Jul 29.
Artigo em Inglês | MEDLINE | ID: mdl-35856849

RESUMO

A Ni-catalyzed reductive arylalkenylation of alkynes with 1-bromo-2-(2-chlorovinyl)arenes in the presence of zinc powder has been developed. This base-free cyclization provides a novel protocol for the selective synthesis of 2-trifluoromethyl naphthalenes and ethyl 2-naphthoates from simple starting materials in moderate to good yields with excellent tolerance of functional groups.

13.
Adv Mater ; 34(29): e2202026, 2022 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-35661432

RESUMO

Multiplexing technology with increased information capacity plays a crucial role in the realm of acoustic communication. Different quantities of sound waves, including time, frequency, amplitude, phase, and orbital angular momentum (OAM), have been independently introduced as the physical multiplexing approach to allow for enhanced communication densities. An acoustic metasurface is decorated with carbon nanotube patches, which when electrically pumped and set to rotate, functions as a hybrid mode-frequency-division multiplexer with synthetic dimensions. Based on this spatiotemporal modulation, a superposition of vortex beams with orthogonal OAMs and symmetric harmonics are both numerically and experimentally demonstrated. Also, flexible combinations of OAM modes with diverse frequency shifts are obtained by transforming the azimuthal phase distributions, which inspires a mode-frequency-division multiplexing approach that significantly promotes the communication capacity.

14.
Chem Asian J ; 14(23): 4358-4364, 2019 Dec 02.
Artigo em Inglês | MEDLINE | ID: mdl-31680431

RESUMO

A convenient and effective protocol for the synthesis of 3-sulfonated quinolines via copper-catalyzed electrophilic cyclization of N-propargylamines has been developed, in which cheap and stable sodium sulfinates were utilized as green sulfonylation reagents. This cascade transformation involves radical addition, cyclization and dehydrogenative aromatization processes in a one-pot reaction under mild conditions.

15.
Chem Commun (Camb) ; 51(6): 1012-5, 2015 Jan 21.
Artigo em Inglês | MEDLINE | ID: mdl-25493628

RESUMO

A new strategy for the synthesis of epoxides is presented. This process allows the direct synthesis of epoxides from alkenes and aldehydes through C-H functionalization and C-C/C-O bond formation.

16.
Chem Commun (Camb) ; 51(85): 15558-61, 2015 Nov 04.
Artigo em Inglês | MEDLINE | ID: mdl-26352340

RESUMO

A copper and iodine-mediated C-H oxidative sulfenylation of olefins with diaryl disulfides has been developed for the stereospecific synthesis of vinyl thioether. With the combination of Cu(OTf)2 and I2, a variety of terminal alkenes underwent oxidative coupling reaction with various diaryl disulfides successfully to afford the corresponding E-vinyl sulfides in moderate to good yields.


Assuntos
Alcenos/química , Cobre/química , Sulfetos/química , Sulfetos/síntese química , Iodo/química , Estrutura Molecular , Oxirredução , Estereoisomerismo
17.
Chem Commun (Camb) ; 50(93): 14554-7, 2014 Dec 04.
Artigo em Inglês | MEDLINE | ID: mdl-25308914

RESUMO

A novel one-pot strategy for the synthesis of 3-trifluoromethylquinoxalines from N-aryl enamines and nitromethane was developed. The tandem reaction is achieved through nitrosation of alkenes, tautomerization and cyclization, which can be applicable to a wide range of enamines with excellent functional group tolerance and afford quinoxalines in moderate to good yields.


Assuntos
Aminas/química , Metano/análogos & derivados , Nitroparafinas/química , Quinoxalinas/síntese química , Ciclização , Metano/química , Estrutura Molecular , Nitrosação , Oxirredução , Quinoxalinas/química
18.
Plant Cell Physiol ; 47(9): 1274-84, 2006 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-16926166

RESUMO

The best known property of plant proteinase inhibitor II (PIN2) genes is their wound-inducible expression in leaves and constitutive expression in flowers. Here we show by promoter analysis in transgenic plants and in situ reverse transcription-PCR (RT-PCR) analysis that SaPIN2b, a member of the PIN2 gene family of nightshade (Solanum americanum), is also constitutively expressed in glandular trichomes. SaPIN2b promoter and its deletions were cloned and fused upstream of beta-glucuronidase (GUS) to transform the nightshade and tobacco (Nicotiana tabacum) plants. Histochemical staining assays indicated that SaPIN2b:GUS was expressed constitutively in glandular trichomes, predominantly in the gland cells, of both transgenic nightshade and tobacco plants. Constitutive expression of SaPIN2b in glandular trichomes was further confirmed by liquid phase in situ RT-PCR analysis of nightshade leaves. Deletion analysis from the 5' end of the SaPIN2b promoter revealed that separate regulatory elements control SaPIN2b expression in gland cells and stalk cells of glandular trichomes. Fluorometric GUS assays showed that SaPIN2b:GUS expression was significantly increased in transgenic plant leaves after mechanical wounding or methyl jasmonate treatment. The SaPIN2b promoter sequence contains six MYB-binding motifs and an L1 box that are involved in trichome differentiation and development. Overexpression of SaPIN2b in tobacco resulted in a significant increase in glandular trichome density and promotion of trichome branching. These results suggest that, as well as being an induced defensive protein of the well-known PIN2 family, SaPIN2b could also play roles in trichome-based defense by functioning as a constitutive component of trichome chemical defense and/or by regulating the development of glandular trichomes.


Assuntos
Proteínas de Plantas/genética , Solanum/genética , Acetatos/farmacologia , Sequência de Bases , Clonagem Molecular , Ciclopentanos/farmacologia , Regulação da Expressão Gênica de Plantas/efeitos dos fármacos , Genes de Plantas , Dados de Sequência Molecular , Oxilipinas , Plantas Geneticamente Modificadas , Regiões Promotoras Genéticas , RNA Mensageiro/genética , RNA Mensageiro/metabolismo , RNA de Plantas/genética , RNA de Plantas/metabolismo , Reação em Cadeia da Polimerase Via Transcriptase Reversa , Solanum/metabolismo , Nicotiana/genética
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