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1.
Nature ; 605(7909): 262-267, 2022 05.
Artículo en Inglés | MEDLINE | ID: mdl-35546188

RESUMEN

The scaling of silicon metal-oxide-semiconductor field-effect transistors has followed Moore's law for decades, but the physical thinning of silicon at sub-ten-nanometre technology nodes introduces issues such as leakage currents1. Two-dimensional (2D) layered semiconductors, with an atomic thickness that allows superior gate-field penetration, are of interest as channel materials for future transistors2,3. However, the integration of high-dielectric-constant (κ) materials with 2D materials, while scaling their capacitance equivalent thickness (CET), has proved challenging. Here we explore transferrable ultrahigh-κ single-crystalline perovskite strontium-titanium-oxide membranes as a gate dielectric for 2D field-effect transistors. Our perovskite membranes exhibit a desirable sub-one-nanometre CET with a low leakage current (less than 10-2 amperes per square centimetre at 2.5 megavolts per centimetre). We find that the van der Waals gap between strontium-titanium-oxide dielectrics and 2D semiconductors mitigates the unfavourable fringing-induced barrier-lowering effect resulting from the use of ultrahigh-κ dielectrics4. Typical short-channel transistors made of scalable molybdenum-disulfide films by chemical vapour deposition and strontium-titanium-oxide dielectrics exhibit steep subthreshold swings down to about 70 millivolts per decade and on/off current ratios up to 107, which matches the low-power specifications suggested by the latest International Roadmap for Devices and Systems5.

2.
J Am Chem Soc ; 146(22): 15198-15208, 2024 Jun 05.
Artículo en Inglés | MEDLINE | ID: mdl-38743271

RESUMEN

Various monovalent cations are employed to construct metal halide perovskites with various structures and functionalities. However, perovskites based on highly polar A-site cations have seldom been reported. Here, a novel hybrid 0D (NH4)x(OH3)3-xInCl6 perovskite with highly polar hydronium OH3+ cations is introduced in this study. Upon doping with Sb3+, hybrid 0D (NH4)x(OH3)3-xInCl6 single crystals exhibited highly efficient broadband yellowish-green (550 nm) and red (630 nm) dual emissions with a PLQY of 86%. The dual emission arises due to Sb3+ occupying two sites within the crystal lattice that possess different polarization environments, leading to distinct Stokes shift energies. The study revealed that lattice polarity plays a significant role in the self-trapped exciton emission of Sb3+-doped perovskites, contributing up to 25% of the Stokes shift energy for hybrid 0D (NH4)x(OH3)3-xInCl6:Sb3+ as a secondary source, in addition to the Jahn-Teller deformation. These findings highlight the potential of Sb3+-doped perovskites for achieving tunable broadband emission and underscore the importance of lattice polarity in determining the emission properties of perovskite materials.

3.
Proc Natl Acad Sci U S A ; 118(13)2021 03 30.
Artículo en Inglés | MEDLINE | ID: mdl-33753481

RESUMEN

The CXC chemokine receptor type 4 (CXCR4) receptor and its ligand, CXCL12, are overexpressed in various cancers and mediate tumor progression and hypoxia-mediated resistance to cancer therapy. While CXCR4 antagonists have potential anticancer effects when combined with conventional anticancer drugs, their poor potency against CXCL12/CXCR4 downstream signaling pathways and systemic toxicity had precluded clinical application. Herein, BPRCX807, known as a safe, selective, and potent CXCR4 antagonist, has been designed and experimentally realized. In in vitro and in vivo hepatocellular carcinoma mouse models it can significantly suppress primary tumor growth, prevent distant metastasis/cell migration, reduce angiogenesis, and normalize the immunosuppressive tumor microenvironment by reducing tumor-associated macrophages (TAMs) infiltration, reprogramming TAMs toward an immunostimulatory phenotype and promoting cytotoxic T cell infiltration into tumor. Although BPRCX807 treatment alone prolongs overall survival as effectively as both marketed sorafenib and anti-PD-1, it could synergize with either of them in combination therapy to further extend life expectancy and suppress distant metastasis more significantly.


Asunto(s)
Antineoplásicos/farmacología , Protocolos de Quimioterapia Combinada Antineoplásica/farmacología , Carcinoma Hepatocelular/tratamiento farmacológico , Neoplasias Hepáticas/tratamiento farmacológico , Receptores CXCR4/antagonistas & inhibidores , Animales , Antineoplásicos/uso terapéutico , Protocolos de Quimioterapia Combinada Antineoplásica/uso terapéutico , Carcinoma Hepatocelular/inmunología , Carcinoma Hepatocelular/patología , Línea Celular Tumoral , Dietilnitrosamina/administración & dosificación , Dietilnitrosamina/toxicidad , Sinergismo Farmacológico , Humanos , Neoplasias Hepáticas/inmunología , Neoplasias Hepáticas/patología , Neoplasias Hepáticas Experimentales/inducido químicamente , Neoplasias Hepáticas Experimentales/tratamiento farmacológico , Neoplasias Hepáticas Experimentales/inmunología , Neoplasias Hepáticas Experimentales/patología , Linfocitos Infiltrantes de Tumor/efectos de los fármacos , Linfocitos Infiltrantes de Tumor/inmunología , Masculino , Ratones , Simulación del Acoplamiento Molecular , Ratas , Receptores CXCR4/metabolismo , Transducción de Señal/efectos de los fármacos , Sorafenib/farmacología , Sorafenib/uso terapéutico , Linfocitos T Citotóxicos/efectos de los fármacos , Linfocitos T Citotóxicos/inmunología , Microambiente Tumoral/efectos de los fármacos , Microambiente Tumoral/inmunología , Macrófagos Asociados a Tumores/efectos de los fármacos , Macrófagos Asociados a Tumores/inmunología , Macrófagos Asociados a Tumores/metabolismo , Ensayos Antitumor por Modelo de Xenoinjerto
4.
Small ; 18(38): e2203311, 2022 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-35989093

RESUMEN

Metal-halide perovskites have drawn profuse attention during the past decade, owing to their excellent electrical and optical properties, facile synthesis, efficient energy conversion, and so on. Meanwhile, the development of information storage technologies and digital communications has fueled the demand for novel semiconductor materials. Low-dimensional perovskites have offered a new force to propel the developments of the memory field due to the excellent physical and electrical properties associated with the reduced dimensionality. In this review, the mechanisms, properties, as well as stability and performance of low-dimensional perovskite memories, involving both molecular-level perovskites and structure-level nanostructures, are comprehensively reviewed. The property-performance correlation is discussed in-depth, aiming to present effective strategies for designing memory devices based on this new class of high-performance materials. Finally, the existing challenges and future opportunities are presented.

5.
Angew Chem Int Ed Engl ; 59(16): 6540-6545, 2020 04 16.
Artículo en Inglés | MEDLINE | ID: mdl-31944523

RESUMEN

The cross-conjugated vinylogous [4+2] anionic annulation has been newly developed, the cascade process of which has a high preference for regiochemical control and chemoselectivity, giving rise to exclusively Michael-type adducts in moderate to high yields (up to 94 %, 35 examples). By making use of this approach as a key operation, the first total synthesis of natural antibiotic ABX, in racemic form, has been successfully achieved in a concise 7-step sequence with an overall yield of about 20 %.


Asunto(s)
Antibacterianos/síntesis química , Productos Biológicos/química , Aniones/química , Antibacterianos/química , Productos Biológicos/síntesis química , Reacción de Cicloadición , Estereoisomerismo
6.
Bioorg Med Chem ; 27(1): 216-223, 2019 01 01.
Artículo en Inglés | MEDLINE | ID: mdl-30528163

RESUMEN

The [18F] isotope-labelled CB1 inverse agonist 3 was elaborated and synthesized for positron emission tomography scanning studies. After immediate purification and calibration with its unlabeled counterpart, compound 3 was intravenously injected in mice and revealed that its distribution percentage in brain over 90-min scans among five region of interests, including brain, liver, heart, thigh muscle and kidney was lower than 1%, thus providing direct evidence to justify itself as a peripherally restricted CB1 antagonist.


Asunto(s)
Agonistas de Receptores de Cannabinoides/farmacología , Pirazoles/farmacología , Receptor Cannabinoide CB1/agonistas , Sulfonamidas/farmacología , Tiofenos/farmacología , Animales , Agonistas de Receptores de Cannabinoides/síntesis química , Agonistas de Receptores de Cannabinoides/química , Agonistas de Receptores de Cannabinoides/farmacocinética , Agonismo Inverso de Drogas , Radioisótopos de Flúor , Marcaje Isotópico , Masculino , Ratones Endogámicos C57BL , Tomografía de Emisión de Positrones/métodos , Pirazoles/síntesis química , Pirazoles/química , Pirazoles/farmacocinética , Receptor Cannabinoide CB1/antagonistas & inhibidores , Sulfonamidas/síntesis química , Sulfonamidas/química , Sulfonamidas/farmacocinética , Tiofenos/química , Tiofenos/farmacocinética , Distribución Tisular
7.
Med Res Rev ; 38(4): 1188-1234, 2018 07.
Artículo en Inglés | MEDLINE | ID: mdl-28768055

RESUMEN

CXCR4 antagonists (e.g., PlerixaforTM ) have been successfully validated as stem cell mobilizers for peripheral blood stem cell transplantation. Applications of the CXCR4 antagonists have heralded the era of cell-based therapy and opened a potential therapeutic horizon for many unmet medical needs such as kidney injury, ischemic stroke, cancer, and myocardial infarction. In this review, we first introduce the central role of CXCR4 in diverse cellular signaling pathways and discuss its involvement in several disease progressions. We then highlight the molecular design and optimization strategies for targeting CXCR4 from a large number of case studies, concluding that polyamines are the preferred CXCR4-binding ligands compared to other structural options, presumably by mimicking the highly positively charged natural ligand CXCL12. These results could be further justified with computer-aided docking into the CXCR4 crystal structure wherein both major and minor subpockets of the binding cavity are considered functionally important. Finally, from the clinical point of view, CXCR4 antagonists could mobilize hematopoietic stem/progenitor cells with long-term repopulating capacity to the peripheral blood, promising to replace surgically obtained bone marrow cells as a preferred source for stem cell transplantation.


Asunto(s)
Quimiocina CXCL12/química , Infecciones por VIH/tratamiento farmacológico , Movilización de Célula Madre Hematopoyética , Células Madre Hematopoyéticas/citología , Receptores CXCR4/antagonistas & inhibidores , Animales , Enfermedades Autoinmunes/tratamiento farmacológico , Ensayos Clínicos como Asunto , Cristalografía por Rayos X , Humanos , Inmunoterapia , Ligandos , Isquemia Miocárdica/tratamiento farmacológico , Metástasis de la Neoplasia , Neutrófilos/citología , Péptidos/química , Regeneración , Transducción de Señal , Trasplante de Células Madre
8.
J Org Chem ; 83(12): 6508-6523, 2018 06 15.
Artículo en Inglés | MEDLINE | ID: mdl-29785848

RESUMEN

Making use of a reductive olefin coupling reaction and Michael-Dieckmann condensation as two key operations, we have completed a concise total synthesis of tetarimycin A, (±)-naphthacemycin A9, and (±)-fasamycin A in a highly convergent and practical protocol. Synthetic procedures thus developed have also been applied to provide related analogues for structure-activity relationship studies, thereby coming to the conclusion that the free hydroxyl group at C-10 is essential for exerting inhibitory activities against a panel of Gram-positive bacteria, including drug-resistant strains VRE and MRSA.


Asunto(s)
Compuestos de Bifenilo/síntesis química , Compuestos de Bifenilo/farmacología , Farmacorresistencia Microbiana/efectos de los fármacos , Bacterias Grampositivas/efectos de los fármacos , Naftacenos/síntesis química , Naftacenos/farmacología , Hidrocarburos Policíclicos Aromáticos/síntesis química , Hidrocarburos Policíclicos Aromáticos/farmacología , Compuestos Policíclicos/síntesis química , Compuestos Policíclicos/farmacología , Relación Estructura-Actividad
9.
J Org Chem ; 81(22): 10759-10768, 2016 11 18.
Artículo en Inglés | MEDLINE | ID: mdl-27750001

RESUMEN

A new N-hydroxyphthalimide (NHPI)/Co(II)-catalyzed protocol, mechanistically involving a sequence of α-hydrogen abstraction, 5-exo-dig cyclization, oxygen capture, hydrogen transfer, and 1,4-dehydration, has been developed to facilitate aerobic oxidation of aryl-, silyl-, and alkyl-capped alkynyl α-cyano alkanone systems to the corresponding highly functionalized products in an effective manner, thus turning this novel chain reaction, originally occurring spontaneously in low yields, into a practical methodology.

10.
Nano Lett ; 13(4): 1852-7, 2013 Apr 10.
Artículo en Inglés | MEDLINE | ID: mdl-23506011

RESUMEN

Recently, monolayers of layered transition metal dichalcogenides (LTMD), such as MX2 (M = Mo, W and X = S, Se), have been reported to exhibit significant spin-valley coupling and optoelectronic performances because of the unique structural symmetry and band structures. Monolayers in this class of materials offered a burgeoning field in fundamental physics, energy harvesting, electronics, and optoelectronics. However, most studies to date are hindered by great challenges on the synthesis and transfer of high-quality LTMD monolayers. Hence, a feasible synthetic process to overcome the challenges is essential. Here, we demonstrate the growth of high-quality MS2 (M = Mo, W) monolayers using ambient-pressure chemical vapor deposition (APCVD) with the seeding of perylene-3,4,9,10-tetracarboxylic acid tetrapotassium salt (PTAS). The growth of a MS2 monolayer is achieved on various surfaces with a significant flexibility to surface corrugation. Electronic transport and optical performances of the as-grown MS2 monolayers are comparable to those of exfoliated MS2 monolayers. We also demonstrate a robust technique in transferring the MS2 monolayer samples to diverse surfaces, which may stimulate the progress on the class of materials and open a new route toward the synthesis of various novel hybrid structures with LTMD monolayer and functional materials.


Asunto(s)
Disulfuros/química , Metales/química , Nanotecnología , Electrónica , Perileno/química , Propiedades de Superficie
11.
Nat Nanotechnol ; 2024 Jun 21.
Artículo en Inglés | MEDLINE | ID: mdl-38907040

RESUMEN

Researchers have been developing 2D materials (2DM) for electronics, which are widely considered a possible replacement for silicon in future technology. Two-dimensional transition metal dichalcogenides are the most promising among the different materials due to their electronic performance and relatively advanced development. Although field-effect transistors (FETs) based on 2D transition metal dichalcogenides have been found to outperform Si in ultrascaled devices, the comparison of 2DM-based and Si-based technologies at the circuit level is still missing. Here we compare 2DM- and Si FET-based static random-access memory (SRAM) circuits across various technology nodes from 16 nm to 1 nm and reveal that the 2DM-based SRAM exhibits superior performance in terms of stability, operating speed and energy efficiency when compared with Si SRAM. This study utilized technology computer-aided design to conduct device and circuit simulations, employing calibrated MoS2 nFETs and WSe2 pFETs. It incorporated layout design rules across various technology nodes to comprehensively analyse their SRAM functionality. The results show that, compared with three-dimensional structure Si transistors at 1 nm node, the planar 2DMFETs exhibited lower capacitance, leading to reduced cell read access time (-16%), reduced time to write (-72%) and lowered dynamic power (-60%). The study highlights the provisional benefits of using planar 2DM transistors to mitigate the performance degradation caused by reduced metal pitch and increased wire resistance in advanced nodes, potentially opening up exciting possibilities for high-performance and low-power circuit applications.

12.
ACS Appl Mater Interfaces ; 16(22): 28980-28990, 2024 Jun 05.
Artículo en Inglés | MEDLINE | ID: mdl-38768264

RESUMEN

Freestanding single-crystalline SrTiO3 membranes, as high-κ dielectrics, hold significant promise as the gate dielectric in two-dimensional (2D) flexible electronics. Nevertheless, the mechanical properties of the SrTiO3 membranes, such as elasticity, remain a critical piece of the puzzle to adequately address the viability of their applications in flexible devices. Here, we report statistical analysis on plane-strain effective Young's modulus of large-area SrTiO3 membranes (5 × 5 mm2) over a series of thicknesses (from 6.5 to 32.2 nm), taking advantage of a highly efficient buckling-based method, which reveals its evident thickness-dependent behavior ranging from 46.01 to 227.17 GPa. Based on microscopic and theoretical results, we elucidate these thickness-dependent behaviors and statistical data deviation with a bilayer model, which consists of a surface layer and a bulk-like layer. The analytical results show that the ∼3.1 nm surface layer has a significant elastic softening compared to the bulk-like layer, while the extracted modulus of the bulk-like layer shows a variation of ∼40 GPa. This variation is considered as a combined contribution from oxygen deficiency presenting in SrTiO3 membranes, and the alignment between applied strain and the crystal orientation. Upon comparison of the extracted elastic properties and electrostatic control capability to those of other typical gate dielectrics, the superior performance of single-crystalline SrTiO3 membranes has been revealed in the context of flexible gate dielectrics, indicating the significant potential of their application in high-performance flexible 2D electronics.

13.
Small ; 9(19): 3253-8, 2013 Oct 11.
Artículo en Inglés | MEDLINE | ID: mdl-23554324

RESUMEN

Fluorescence quenching microscopy (FQM) is demonstrated as a low-cost and high-throughput technique for seeing graphene-like 2D sheets such as MoS2 . FQM provides high contrast and layer resolution comparable to those of scanning electron microscopy, but allows the imaging of samples deposited on arbitrary substrates, including non-conductive substrates such as quartz. Solution fluorescence quenching studies suggest that FQM should be feasible for many other 2D materials such as WS2 , Bi2 Te3 , MoSe2 , NbSe2 , and TaS2 .


Asunto(s)
Microscopía Fluorescente/métodos
14.
Micromachines (Basel) ; 14(11)2023 Oct 27.
Artículo en Inglés | MEDLINE | ID: mdl-38004849

RESUMEN

Semiconductor materials, devices, and systems have become indispensable pillars supporting the modern world, deeply ingrained in various facets of our daily lives [...].

15.
Micromachines (Basel) ; 14(11)2023 Oct 31.
Artículo en Inglés | MEDLINE | ID: mdl-38004899

RESUMEN

The GaN industry always demands further improvement in the power transport capability of GaN-based high-energy mobility transistors (HEMT). This paper presents a novel enhancement-type GaN HEMT with high power transmission capability, which utilizes a coherent channel that can form a three-dimensional electron sea. The proposed device is investigated using the Silvaco simulation tool, which has been calibrated against experimental data. Numerical simulations prove that the proposed device has a very high on-state current above 3 A/mm, while the breakdown voltage (above 800 V) is not significantly affected. The calculated Johnson's and Baliga's figure-of-merits highlight the promise of using such a coherent channel for enhancing the performance of GaN HEMTs in power electronics applications.

16.
Adv Sci (Weinh) ; 10(7): e2205809, 2023 03.
Artículo en Inglés | MEDLINE | ID: mdl-36698305

RESUMEN

Solar-driven photothermal water evaporation is considered an elegant and sustainable technology for freshwater production. The existing systems, however, often suffer from poor stability and biofouling issues, which severely hamper their prospects in practical applications. Conventionally, photothermal materials are deposited on the membrane supports via vacuum-assisted filtration or dip-coating methods. Nevertheless, the weak inherent material-membrane interactions frequently lead to poor durability, and the photothermal material layer can be easily peeled off from the hosting substrates or partially dissolved when immersed in water. In the present article, the discovery of the incorporation of borophene into cellulose nanofibers (CNF), enabling excellent environmental stability with a high light-to-heat conversion efficiency of 91.5% and water evaporation rate of 1.45 kg m-2 h-1 under simulated sunlight is reported. It is also demonstrated that borophene papers can be employed as an excellent active photothermal material for eliminating almost 100% of both gram-positive and gram-negative bacteria within 20 min under three sun irradiations. The result opens a new direction for the design of borophene-based papers with unique photothermal properties which can be used for the effective treatment of a wide range of wastewaters.


Asunto(s)
Bacterias Gramnegativas , Agua , Antibacterianos , Bacterias Grampositivas , Celulosa
17.
Adv Mater ; 34(18): e2108616, 2022 May.
Artículo en Inglés | MEDLINE | ID: mdl-34995372

RESUMEN

Contact engineering is a prerequisite for achieving desirable functionality and performance of semiconductor electronics, which is particularly critical for organic-inorganic hybrid halide perovskites due to their ionic nature and highly reactive interfaces. Although the interfaces between perovskites and charge-transporting layers have attracted lots of attention due to the photovoltaic and light-emitting diode applications, achieving reliable perovskite/electrode contacts for electronic devices, such as transistors and memories, remains as a bottleneck. Herein, a critical review on the elusive nature of perovskite/electrode interfaces with a focus on the interfacial electrochemistry effects is presented. The basic guidelines of electrode selection are given for establishing non-polarized interfaces and optimal energy level alignment for perovskite materials. Furthermore, state-of-the-art strategies on interface-related electrode engineering are reviewed and discussed, which aim at achieving ohmic transport and eliminating hysteresis in perovskite devices. The role and multiple functionalities of self-assembled monolayers that offer a unique approach toward improving perovskite/electrode contacts are also discussed. The insights on electrode engineering pave the way to advancing stable and reliable perovskite devices in diverse electronic applications.

18.
Nat Commun ; 13(1): 4149, 2022 Jul 18.
Artículo en Inglés | MEDLINE | ID: mdl-35851038

RESUMEN

Two-dimensional (2D) semiconducting monolayers such as transition metal dichalcogenides (TMDs) are promising channel materials to extend Moore's Law in advanced electronics. Synthetic TMD layers from chemical vapor deposition (CVD) are scalable for fabrication but notorious for their high defect densities. Therefore, innovative endeavors on growth reaction to enhance their quality are urgently needed. Here, we report that the hydroxide W species, an extremely pure vapor phase metal precursor form, is very efficient for sulfurization, leading to about one order of magnitude lower defect density compared to those from conventional CVD methods. The field-effect transistor (FET) devices based on the proposed growth reach a peak electron mobility ~200 cm2/Vs (~800 cm2/Vs) at room temperature (15 K), comparable to those from exfoliated flakes. The FET device with a channel length of 100 nm displays a high on-state current of ~400 µA/µm, encouraging the industrialization of 2D materials.

19.
Org Lett ; 23(15): 5709-5713, 2021 Aug 06.
Artículo en Inglés | MEDLINE | ID: mdl-34289688

RESUMEN

Anionic Diels-Alder chemistry of electron-deficient cross-conjugated vinylogous alkenones, providing highly stable sodium dienolate ion pairs as electron-rich dienes in the presence of a weak sodium base in THF, has been newly developed, leading to a single Diels-Alder adduct, in racemic form, in moderate to high yields (up to 97%, 37 examples).

20.
ACS Appl Mater Interfaces ; 13(40): 47962-47971, 2021 Oct 13.
Artículo en Inglés | MEDLINE | ID: mdl-34591469

RESUMEN

Two-dimensional transition metal dichalcogenide (TMDC) nanocrystals (NCs) exhibit unique optical and electrocatalytic properties. However, the growth of uniform and high-quality NCs of monolayer TMDC remains a challenge. Until now, most of them are synthesized via a solution-based hydrothermal process or ultrasonic exfoliation method, in which the capping ligands introduced from organic solution often quench the optical and electrocatalytic properties of TMDC NCs. Moreover, it is difficult to homogeneously disperse the solution-based TMDC NCs on a substrate for device fabrication, since the dispersed NCs can easily aggregate. Here, we put forward a novel CVD method to grow closely spaced MoS2 NCs around 5 nm in lateral size. TEM and AFM characterizations demonstrate the monolayer and high-crystalline nature of MoS2 NCs. An obvious blue-shift with 130 meV in photoluminescence signals can be observed. The MoS2 NCs also show an outstanding surface-enhanced Raman scattering for organic molecules due to their localized surface plasmon and abundant edge sites and exhibit excellent electrocatalytic properties for the hydrogen-evolution reaction with a very low onset potential of ∼50 mV and Tafel slope of ∼57 mV/decade. Finally, we further demonstrate this kind of CVD method as a versatile platform for the growth of other TMDC NCs, such as WSe2 and MoSe2 NCs.

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