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1.
Sci Adv ; 9(49): eadj3955, 2023 Dec 08.
Artigo em Inglês | MEDLINE | ID: mdl-38064554

RESUMO

The discovery of magnetism in van der Waals (vdW) materials has established unique building blocks for the research of emergent spintronic phenomena. In particular, owing to their intrinsically clean surface without dangling bonds, the vdW magnets hold the potential to construct a superior interface that allows for efficient electrical manipulation of magnetism. Despite several attempts in this direction, it usually requires a cryogenic condition and the assistance of external magnetic fields, which is detrimental to the real application. Here, we fabricate heterostructures based on Fe3GaTe2 flakes that have room-temperature ferromagnetism with excellent perpendicular magnetic anisotropy. The current-driven nonreciprocal modulation of coercive fields reveals a high spin-torque efficiency in the Fe3GaTe2/Pt heterostructures, which further leads to a full magnetization switching by current. Moreover, we demonstrate the field-free magnetization switching resulting from out-of-plane polarized spin currents by asymmetric geometry design. Our work could expedite the development of efficient vdW spintronic logic, memory, and neuromorphic computing devices.

2.
ACS Appl Mater Interfaces ; 15(42): 49362-49369, 2023 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-37826857

RESUMO

Piezoelectric sensors are excellent damage detectors that can be applied to structural health monitoring (SHM). SHM for complex structures of aerospace vehicles working in harsh conditions is frequently required, posing challenging requirements for a sensor's flexibility, radiation hardness, and high-temperature tolerance. Here, we fabricate a flexible and lightweight Pb(Zr0.53Ti0.47)O3 piezoelectric film on flexible KMg3(AlSi3O10)F2 substrate via van der Waals (vdW) heteroepitaxy, endowing it with robust ferroelectric and piezoelectric properties under low energy-high flux protons (LE-HFPs) radiation (1015 p/cm2). More importantly, the Pb(Zr0.53Ti0.47)O3 film sensor maintains highly stable damage monitoring sensitivity on an aluminum plate under harsh conditions of LE-HFPs radiation (1015 p/cm2, flat structure), high temperature (175 °C, flat structure), and mechanical fatigue (bending 105 cycles under a radius of 5 mm, curved structure). All these superior qualities are suggested to result from the outstanding film crystal quality due to vdW epitaxy. The flexible and lightweight Pb(Zr0.53Ti0.47)O3 film sensor demonstrated in this work provides an ideal candidate for real-time SHM of aerospace vehicles with flat and complex curve-like structures working in harsh aerospace environments.

3.
J Am Chem Soc ; 145(20): 10998-11004, 2023 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-37167083

RESUMO

The first total synthesis of (±)- and (-)-daphnillonin B, a daphnicyclidin-type alkaloid with a new [7-6-5-7-5-5] A/B/C/D/E/F hexacyclic core, has been achieved. The [6-5-7] B/C/D ring system was efficiently and diastereoselectively constructed via a mild type I intramolecular [5+2] cycloaddition, followed by a Grubbs II catalyst-catalyzed radical cyclization. The [5-5] fused E/F ring system was synthesized via a diastereoselective intramolecular Pauson-Khand reaction. Notably, the synthetically challenging [7-6-5-7-5-5] hexacyclic core was reassembled by a unique Wagner-Meerwein-type rearrangement from the [6-6-5-7-5-5] hexacyclic framework found in calyciphylline A-type Daphniphyllum alkaloids.

4.
Small ; 19(30): e2300824, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37060220

RESUMO

Complex oxide films stabilized by epitaxial growth can exhibit large populations of point defects which have important effects on their properties. The site occupancy of pulsed laser-deposited epitaxial terbium iron garnet (TbIG) films with excess terbium (Tb) is analyzed, in which the terbium:iron (Tb:Fe)ratio is 0.86 compared to the stoichiometric value of 0.6. The magnetic properties of the TbIG are sensitive to site occupancy, exhibiting a higher compensation temperature (by 90 K) and a lower Curie temperature (by 40 K) than the bulk Tb3 Fe5 O12 garnet. Data derived from X-ray core-level spectroscopy, magnetometry, and molecular field coefficient modeling are consistent with occupancy of the dodecahedral sites by Tb3+ , the octahedral sites by Fe3+ , Tb3+ and vacancies, and the tetrahedral sites by Fe3+ and vacancies. Energy dispersive X-ray spectroscopy in a scanning transmission electron microscope provides direct evidence of TbFe antisites. A small fraction of Fe2+ is present, and oxygen vacancies are inferred to be present to maintain charge neutrality. Variation of the site occupancies provides a path to considerable manipulation of the magnetic properties of epitaxial iron garnet films and other complex oxides, which readily accommodate stoichiometries not found in their bulk counterparts.

5.
J Med Chem ; 2022 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-35852796

RESUMO

Inhibition of autophagy has been widely viewed as a promising strategy for anticancer therapy. However, few effective and specific autophagy inhibitors have been reported. Herein, we described the design, synthesis, and biological characteristics of new analogues of strigolactones (SLs), an emerging class of plant hormones, against colorectal cancers. Among them, an enantiopure analogue 6 exerted potent and selective cytotoxicity against colorectal cancer cells, but not normal human colon mucosal epithelial cells, which were further confirmed by the plate colony formation assay. Moreover, it significantly inhibited tumor growth in an HCT116 xenograft mouse model with low toxicity. Mechanistically, it is associated with selective induction of cell apoptosis and cell cycle arrest. Remarkably, 6 acted as a potent autophagy/mitophagy inhibitor by selectively increasing the autophagic flux while blocking the autophagosome-lysosome fusion in HCT116 cells. This study features stereo-defined SLs as novel autophagy inhibitors with high cancer cell specificity, which paves a new path for anticolorectal cancer therapy.

6.
Nat Commun ; 12(1): 4298, 2021 Jul 14.
Artigo em Inglês | MEDLINE | ID: mdl-34262033

RESUMO

Single-phase multiferroic materials that allow the coexistence of ferroelectric and magnetic ordering above room temperature are highly desirable, motivating an ongoing search for mechanisms for unconventional ferroelectricity in magnetic oxides. Here, we report an antisite defect mechanism for room temperature ferroelectricity in epitaxial thin films of yttrium orthoferrite, YFeO3, a perovskite-structured canted antiferromagnet. A combination of piezoresponse force microscopy, atomically resolved elemental mapping with aberration corrected scanning transmission electron microscopy and density functional theory calculations reveals that the presence of YFe antisite defects facilitates a non-centrosymmetric distortion promoting ferroelectricity. This mechanism is predicted to work analogously for other rare earth orthoferrites, with a dependence of the polarization on the radius of the rare earth cation. Our work uncovers the distinctive role of antisite defects in providing a mechanism for ferroelectricity in a range of magnetic orthoferrites and further augments the functionality of this family of complex oxides for multiferroic applications.

7.
ACS Nano ; 14(7): 8949-8957, 2020 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-32568512

RESUMO

Searching for new materials and phenomena to enable voltage control of magnetism and magnetic properties holds compelling interest for the development of low-power nonvolatile memory devices. In particular, reversible and nonvolatile ON/OFF controls of magnetism above room temperature are highly desirable yet still elusive. Here, we report on a nonvolatile voltage control of magnetism in epitaxial SrCo1-xFexO3-δ (SCFO). The substitution of Co with Fe significantly changes the magnetic properties of SCFO. In particular, for the Co/Fe ratio of ∼1:1, a switch between nonmagnetic (OFF) and ferromagnetic (ON) states with a Curie temperature above room temperature is accomplished by ionic liquid gating at ambient conditions with voltages as low as ±2 V, even for films with thickness up to 150 nm. Tuning the oxygen stoichiometry via the polarity and duration of gating enables reversible and continuous control of the magnetization between 0 and 100 emu/cm3 (0.61 µB/f.u.) at room temperature. In addition, SCFO was successfully incorporated into self-assembled two-phase vertically aligned nanocomposites, in which the reversible voltage control of magnetism above room temperature is also attained. The notable structural response of SCFO to ionic liquid gating allows large strain couplings between the two oxides in these nanocomposites, with potential for voltage-controlled and strain-mediated functionality based on couplings between structure, composition, and physical properties.

8.
Org Biomol Chem ; 18(26): 4956-4961, 2020 07 08.
Artigo em Inglês | MEDLINE | ID: mdl-32579656

RESUMO

A highly efficient and modular synthesis of nematode pheromone ascarosides was developed, which highlights a 4-step scalable synthesis of the common intermediate 10 in 23% yield from commercially available l-rhamnose by using orthoesterification/benzylation/orthoester rearrangement as the key step. Six diverse ascarosides were synthesized accordingly. Notably, biological investigations revealed that ascr#1 and ascr#18 treatment resulted in enhanced callose accumulation in Arabidopsis leaves. And ascr#18 also increased the expression of defense-related genes such as PR1, PDF1.2, LOX2 and AOS, which might contribute to the enhanced plant defense responses. This study not only allows a facile access to 1-O, 2-O, and 4-O substituted ascarosides, but also provides valuable insights into their biological activities in inducing plant defense response, as well as their mode of action.


Assuntos
Proteínas de Arabidopsis/metabolismo , Arabidopsis/metabolismo , Glicosídeos/metabolismo , Feromônios/metabolismo , Folhas de Planta/metabolismo , Animais , Arabidopsis/química , Proteínas de Arabidopsis/química , Proteínas de Arabidopsis/genética , Glicosídeos/síntese química , Glicosídeos/química , Conformação Molecular , Nematoides , Feromônios/química , Folhas de Planta/química
9.
Org Lett ; 21(21): 8700-8704, 2019 11 01.
Artigo em Inglês | MEDLINE | ID: mdl-31609125

RESUMO

Psiguajdianone (1), a novel caryophyllene-derived meroterpenoid dimer, was isolated from Psidium guajava. The structure of 1 was determined by X-ray analysis and confirmed by total synthesis. Our synthetic strategy involves biomimetic cascade Knoevenagel condensation/hetero-Diels-Alder reaction and dimerization. Notably, the caryophyllene-derived meroterpenoids obtained during our synthesis were first identified as artifacts in the laboratory, and five of them were proven to be natural products present in the plant. Moreover, these compounds show significant anti-inflammatory activity.


Assuntos
Biomimética , Psidium/química , Terpenos/química , Terpenos/síntese química , Técnicas de Química Sintética
10.
Adv Mater ; 31(43): e1903738, 2019 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-31517407

RESUMO

Lattice defects typically reduce lattice thermal conductivity, which has been widely exploited in applications such as thermoelectric energy conversion. Here, an anomalous dependence of the lattice thermal conductivity on point defects is demonstrated in epitaxial WO3 thin films. Depending on the substrate, the lattice of epitaxial WO3 expands or contracts as protons are intercalated by electrolyte gating or oxygen vacancies are introduced by adjusting growth conditions. Surprisingly, the observed lattice volume, instead of the defect concentration, plays the dominant role in determining the thermal conductivity. In particular, the thermal conductivity increases significantly with proton intercalation, which is contrary to the expectation that point defects typically lower the lattice thermal conductivity. The thermal conductivity can be dynamically varied by a factor of ≈1.7 via electrolyte gating, and tuned over a larger range, from 7.8 to 1.1 W m-1 K-1 , by adjusting the oxygen pressure during film growth. The electrolyte-gating-induced changes in thermal conductivity and lattice dimensions are reversible through multiple cycles. These findings not only expand the basic understanding of thermal transport in complex oxides, but also provide a path to dynamically control the thermal conductivity.

11.
Nanoscale ; 9(31): 11047-11054, 2017 Aug 10.
Artigo em Inglês | MEDLINE | ID: mdl-28604899

RESUMO

The importance of tuning refractive index in a multilayer antireflection coating (ARC) system can not be denied. In practical applications, regulation of refractive index is complex due to limited choice and availability of appropriate materials for the trilayer AR coating assembly. To overcome this issue, we used a single inorganic material, HfO2, for the construction of a trilayer AR light harvesting moth eye, resembling hierarchical nanostructure coatings, for exploring new generation photovoltaics and optoelectronic devices. In the trilayer AR HfO2 (TAR-H) assembly, using a glancing angle deposition technique (GLAD), the dense bottom layer was steadily changed into a spongy middle layer that further changed to a highly porous top layer micmiking a moth eye, reducing the refractive index of the coating from 1.87 to 1.30. The broadband omnidirectional properties of the TAR-H coating, with superior thermal stability and improved scratch resistance, in the visible wavelength range were experimentally demonstrated. The TAR-H coating on FTO and sapphire substrates achieved reflectance of up to <1% in the visible wavelength range.

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