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1.
Adv Sci (Weinh) ; : e2402272, 2024 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-38639395

RESUMO

Here, a photocatalytic asymmetric multicomponent cascade Minisci reaction of ß-carbolines with enamides and diazo compounds is reported, enabling an effective enantioselective radical C─H functionalization of ß-carbolines with high yields and enantioselectivity (up to 83% yield and 95% ee). This enantioselective multicomponent Minisci protocol exhibits step economy, high chemo-/enantio-selective control, and good functional group tolerance, allowing access to a variety of valuable chiral ß-carbolines. Notably, diazo compounds are suitable radical precursors in enantioselective cascade radical reactions. Moreover, the efficiency and practicality of this approach are demonstrated by the asymmetric synthesis of bioactive compounds and natural products.

2.
Nat Mater ; 2024 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-38605194

RESUMO

Magnetic skyrmions are promising as next-generation information units. Their antiparticle-the antiskyrmion-has also been discovered in chiral magnets. Here we experimentally demonstrate antiskyrmion sliding in response to a pulsed electric current at room temperature without the requirement of an external magnetic field. This is realized by embedding antiskyrmions in helical stripe domains, which naturally provide one-dimensional straight tracks along which antiskyrmion sliding can be easily launched with low current density and without transverse deflection from the antiskyrmion Hall effect. The higher mobility of the antiskyrmions in the background of helical stripes in contrast to the typical ferromagnetic state is a result of intrinsic material parameters and elastic energy of the stripe domain, thereby smearing out the random pinning potential, as supported by micromagnetic simulations. The demonstration and comprehensive understanding of antiskyrmion movement along naturally straight tracks offers a new perspective for (anti)skyrmion application in spintronics.

3.
Nat Commun ; 15(1): 3391, 2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38649678

RESUMO

Topological spin textures are characterized by magnetic topological charges, Q, which govern their electromagnetic properties. Recent studies have achieved skyrmion bundles with arbitrary integer values of Q, opening possibilities for exploring topological spintronics based on Q. However, the realization of stable skyrmion bundles in chiral magnets at room temperature and zero magnetic field - the prerequisite for realistic device applications - has remained elusive. Here, through the combination of pulsed currents and reversed magnetic fields, we experimentally achieve skyrmion bundles with different integer Q values - reaching a maximum of 24 at above room temperature and zero magnetic field - in the chiral magnet Co8Zn10Mn2. We demonstrate the field-driven annihilation of high-Q bundles and present a phase diagram as a function of temperature and field. Our experimental findings are consistently corroborated by micromagnetic simulations, which reveal the nature of the skyrmion bundle as that of skyrmion tubes encircled by a fractional Hopfion.

4.
ACS Appl Mater Interfaces ; 16(15): 19112-19120, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38579811

RESUMO

Two-dimensional transition metal dichalcogenide (TMDC) heterostructure is receiving considerable attention due to its novel electronic, optoelectronic, and spintronic devices with design-oriented and functional features. However, direct design and synthesis of high-quality TMDC/MnTe heterostructures remain difficult, which severely impede further investigations of semiconductor/magnetic semiconductor devices. Herein, the synthesis of high-quality vertically stacked WS2/MnTe heterostructures is realized via a two-step chemical vapor deposition method. Raman, photoluminescence, and scanning transmission electron microscopy characterizations reveal the high-quality and atomically sharp interfaces of the WS2/MnTe heterostructure. WS2/MnTe-based van der Waals field effect transistors demonstrate high rectification behavior with rectification ratio up to 106, as well as a typical p-n electrical transport characteristic. Notably, the fabricated WS2/MnTe photodetector exhibits sensitive and broadband photoresponse ranging from UV to NIR with a maximum responsivity of 1.2 × 103 A/W, a high external quantum efficiency of 2.7 × 105%, and fast photoresponse time of ∼50 ms. Moreover, WS2/MnTe heterostructure photodetectors possess a broadband image sensing capability at room temperature, suggesting potential applications in next-generation high-performance and broadband image sensing photodetectors.

5.
J Am Chem Soc ; 146(14): 9768-9778, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38545837

RESUMO

A rhodium-catalyzed 3-component conjunctive diastereo- and regioselective arylamidation of (homo)allylic sulfides, organon boronic acids, and dioxazolones is reported. These reactions deliver the 1,2-insertion and 2,1-insertion arylamidation products, respectively, for allylic sulfides and homoallylic sulfides. The enantioselective arylamidation of terminal and internal allylic sulfides is achieved, furnishing various 1,3-N,S compounds featuring one or two contiguous stereocenters in high yields and with high diastereo- and enantioselectivities. Mechanistic studies suggest a change in the turnover-limiting and selectivity-determining steps induced by the native and easily removable sulfide group.

6.
Small ; : e2311430, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38444270

RESUMO

Effectively tuning magnetic state by using current is essential for novel spintronic devices. Magnetic van der Waals (vdW) materials have shown superior properties for the applications of magnetic information storage based on the efficient spin torque effect. However, for most of known vdW ferromagnets, the ferromagnetic transition temperatures lower than room temperature strongly impede their applications and the room-temperature vdW spintronic device with low energy consumption is still a long-sought goal. Here, the highly efficient room-temperature nonvolatile magnetic switching is realized by current in a single-material device based on vdW ferromagnet Fe3 GaTe2 . Moreover, the switching current density and power dissipation are about 300 and 60000 times smaller than conventional spin-orbit-torque devices of magnet/heavy-metal heterostructures. These findings make an important progress on the applications of magnetic vdW materials in the fields of spintronics and magnetic information storage.

7.
Knee ; 48: 83-93, 2024 Mar 29.
Artigo em Inglês | MEDLINE | ID: mdl-38555717

RESUMO

OBJECTIVE: To investigate the effects of astaxanthin (AST) on mouse osteoarthritis (OA) and lipopolysaccharide (LPS)-induced ATDC5 cell damage and to explore whether SIRT1 protein plays a role. METHODS: In this study, some mouse OA models were constructed by anterior cruciate ligament transection (ACLT). Imaging, molecular biology and histopathology methods were used to study the effect of AST administration on traumatic OA in mice. In addition, LPS was used to stimulate ATDC5 cells to mimic the inflammatory response of OA. The effects of AST on the cell activity, inflammatory cytokines, matrix metalloproteinases and collagen type II levels were studied by CCK8 activity assay, reverse transcription polymerase chain reaction and protein imprinting. The role of SIRT1 protein was also detected. RESULTS: In the mouse OA model, the articular surface collapsed, the articular cartilage thickness and cartilage matrix protein abundance were significantly decreased, while the expression of inflammatory cytokines and matrix metalloproteinases was increased; but AST treatment reversed these effects. Meanwhile, AST pretreatment could partially reverse LPS-induced ATDC5 cell damage and upregulate SIRT1 expression, but this protective effect of AST was attenuated by concurrent administration of the SIRT1 inhibitor Ex527. CONCLUSION: AST can protect against the early stages of OA by affecting SIRT1 signalling, suggesting that AST might be a potential therapeutic agent for OA treatment.

8.
Chem Soc Rev ; 53(7): 3457-3484, 2024 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-38411467

RESUMO

Chiral carbon-carbon (C-C) and carbon-heteroatom (C-X) bonds are pervasive and very essential in natural products, bioactive molecules, and functional materials, and their catalytic construction has emerged as one of the hottest research fields in synthetic organic chemistry. The last decade has witnessed vigorous progress in Rh(I)-catalyzed asymmetric C-H functionalization as a complement to Rh(II) and Rh(III) catalysis. This review aims to provide the most comprehensive and up-to-date summary covering the recent advances in Rh(I)-catalyzed C-H activation for asymmetric functionalization. In addition to the development of diverse reactions, chiral ligand design and mechanistic investigation (inner-sphere mechanism, outer-sphere mechanism, and 1,4-Rh migration) will also be highlighted.

9.
J Am Chem Soc ; 146(8): 5081-5087, 2024 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-38358355

RESUMO

The asymmetric hydrogenation (AH) of N-unprotected indoles is a straightforward, yet challenging method to access biologically interesting NH chiral indolines. This method has for years been limited to 2/3-monosubstituted or 2,3-disubstituted indoles, which produce chiral indolines bearing endocyclic chiral centers. Herein, we have reported an innovative Pd-catalyzed AH of racemic α-alkyl or aryl-substituted indole-2-acetates using an acid-assisted dynamic kinetic resolution (DKR) process, affording a range of structurally fascinating chiral indolines that contain exocyclic stereocenters with excellent yields, diastereoselectivities, and enantioselectivities. Mechanistic studies support that the DKR process relies on a rapid interconversion of each enantiomer of racemic substrates, leveraged by an acid-promoted isomerization between the aromatic indole and nonaromatic exocyclic enamine intermediate. The reaction can be performed on a gram scale, and the products can be derivatized into non-natural ß-amino acids via facile debenzylation and amino alcohol upon reduction.

10.
Adv Mater ; 36(19): e2309538, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38366361

RESUMO

Topological magnetic textures are promising candidates as binary data units for the next-generation memory device. The precise generation and convenient control of nontrivial spin topology at zero field near room temperature endows the critical advantages in skyrmionic devices but is not simultaneously integrated into one material. Here, in the Kagome plane of quantum TbMn6Sn6, the expedient generation of the skyrmion bubbles in versatile forms of lattice, chain, and isolated one by converging the electron beam, where the electron intensity gradient contributes to the dynamic generation from local anisotropy variation near spin reorientation transition (SRT) is reported. Encouragingly, by utilizing the dynamic shift of the SRT domain interface, the straight movement is actualized with the skyrmion bubble slave to the SRT domain interface forming an elastic composite object, avoiding the usual deflection from the skyrmion Hall effect. The critical contribution of the SRT domain interface via conveniently electron-assisted heating is further theoretically validated in micromagnetic simulation, highlighting the compatible application possibility in advanced devices.

11.
Angew Chem Int Ed Engl ; 63(12): e202400502, 2024 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-38279683

RESUMO

Chiral cyclopentadienyl-rhodium(III) Cpx Rh(III) catalysis has been demonstrated to be competent for catalyzing highly enantioselective aziridination of challenging unactivated terminal alkenes and nitrene sources. The chiral Cpx Rh(III) catalysis system exhibited outstanding catalytic performance and wide functional group tolerance, yielding synthetically important and highly valuable chiral aziridines with good to excellent yields and enantioselectivities (up to 99 % yield, 93 % ee). This protocol presents a novel and effective strategy for synthesizing enantioenriched aziridines from simple alkenes. Various transformations were performed on the aziridine products, illustrating the versatility and synthetic potential of this protocol for constructing highly functionalized compounds.

12.
Nanoscale ; 16(3): 1406-1414, 2024 Jan 18.
Artigo em Inglês | MEDLINE | ID: mdl-38165953

RESUMO

Itinerant ferromagnetism at room temperature is a key factor for spin transport and manipulation. Here, we report the realization of near-room temperature itinerant ferromagnetism in Co doped Fe5GeTe2 thin flakes. The ferromagnetic transition temperature TC (∼323 K-337 K) is almost unchanged when the thickness is as low as 12 nm and is still about 284 K at 2 nm (bilayer thickness). Theoretical calculations further indicate that the ferromagnetism persists in monolayer Fe4CoGeTe2. In addition to the robust ferromagnetism down to the ultrathin limit, Fe4CoGeTe2 exhibits an unusual temperature- and thickness-dependent intrinsic anomalous Hall effect. We propose that it could be ascribed to the dependence of the band structure on thickness that changes the Berry curvature near the Fermi energy level subtly. The near-room temperature ferromagnetism and tunable anomalous Hall effect in atomically thin Fe4CoGeTe2 provide opportunities to understand the exotic transport properties of two-dimensional van der Waals magnetic materials and explore their potential applications in spintronics.

13.
BMC Musculoskelet Disord ; 25(1): 56, 2024 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-38216954

RESUMO

BACKGROUND: To analyze the clinical efficacy of K-wire placement guided technology in paediatric supracondylar humerus fractures. METHODS: A retrospective study was conducted in 105 patients who underwent closed reduction and percutaneous pinning surgeries in our hospital from June 2019 to August 2022. 54 patients treated with a assisted reduction fixation device to assist in closed reduction and percutaneous K-wire cross-fixation were allocated into the Non-guided group, and 51 patients with K-wire placement guided technology to guide K-wire placement were assigned into the Guided group. The operation duration, number of disposable K-wire placement, intraoperative fluoroscopy frequency, Baumann angle, carrying angle, fracture healing time and Flynn score of elbow joint function at the final follow-up were compared between two groups. The postoperative complications of two groups were recorded. RESULTS: There were significant differences between two groups in terms of operation duration, intraoperative fluoroscopy frequency, and disposable K-wire placement rate (p < 0. 05), while no significant differences of Baumann angle, carrying angle and the fracture healing time between two groups were observed (p > 0. 05). In the control group, ulnar nerve injury in 2 case, pin site infection in 4 cases, mild cubitus varus in 2 cases and loss of reduction in 4 cases were detected. In the study group, ulnar nerve injury in 1 case, pin site infection in 2 cases and loss of reduction in 1 case was observed. There was no significant difference in Flynn scores between two groups. CONCLUSION: K-wire placement guided technology is simple and convenient. The application of K-wire placement guided technology could relatively improved disposable K-wire placement rate, shorten the intraoperative fluoroscopy frequencies and reduce complication rates.


Assuntos
Fios Ortopédicos , Fraturas do Úmero , Criança , Humanos , Estudos Retrospectivos , Fraturas do Úmero/diagnóstico por imagem , Fraturas do Úmero/cirurgia , Fluoroscopia , Fixação Interna de Fraturas/efeitos adversos , Resultado do Tratamento , Tecnologia , Úmero
14.
Nano Lett ; 24(5): 1587-1593, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38259044

RESUMO

Magnetic skyrmions in bulk materials are typically regarded as two-dimensional structures. However, they also exhibit three-dimensional configurations, known as skyrmion tubes, that elongate and extend in-depth. Understanding the configurations and stabilization mechanism of skyrmion tubes is crucial for the development of advanced spintronic devices. However, the generation and annihilation of skyrmion tubes in confined geometries are still rarely reported. Here, we present direct imaging of skyrmion tubes in nanostructured cuboids of a chiral magnet FeGe using Lorentz transmission electron microscopy (TEM), while applying an in-plane magnetic field. It is observed that skyrmion tubes stabilize in a narrow field-temperature region near the Curie temperature (Tc). Through a field cooling process, metastable skyrmion tubes can exist in a larger region of the field-temperature diagram. Combining these experimental findings with micromagnetic simulations, we attribute these phenomena to energy differences and thermal fluctuations. Our results could promote topological spintronic devices based on skyrmion tubes.

15.
Adv Mater ; 36(14): e2312411, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38155583
17.
ACS Appl Mater Interfaces ; 15(42): 49902-49910, 2023 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-37815887

RESUMO

Electrically generated spin-orbit torque (SOT) has emerged as a powerful pathway to control magnetization for spintronic applications including memory, logic, and neurocomputing. However, the requirement of external magnetic fields, together with the ultrahigh current density, is the main obstacle for practical SOT devices. In this paper, we report that the field-free SOT-driven magnetization switching can be successfully realized by interfacial ion absorption in perpendicular Ta/CoFeB/MgO multilayers. Besides, the tunable SOT efficiency exhibits a strong dependence on interfacial Ti insertion thicknesses. Polarized neutron reflection measurements demonstrate the existence of canted magnetization with Ti inserted, which leads to deterministic magnetization switching. In addition, interfacial characterization and first-principles calculations reveal that B absorption by the Ti layer is the main cause behind the enhanced interfacial transparency, which determines the tunable SOT efficiency. Our findings highlight an attractive scheme to a purely electric control spin configuration, enabling innovative designs for SOT-based spintronics via interfacial engineering.

18.
Adv Mater ; 35(47): e2306117, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37668003

RESUMO

Magnetic skyrmions are spin swirls that possess topological nontriviality and are considered particle-like entities. They are distinguished by an integer topological charge Q. The presence of skyrmion bundles provides an opportunity to explore the range of values for Q, which is crucial for the advancement of topological spintronic devices with multi-Q properties. In this study, a new material candidate, Sr2 Co2 Fe28 O46 hexaferrite of the X-type, which hosts small dipolar skyrmions at room temperature and above is presented. By exploiting reversed magnetic fields from metastable skyrmion bubbles at zero fields, skyrmion-bubble bundles with different interior skyrmion/bubble numbers, topological charges, and morphologies at room temperature are incorporated. These experimental findings are consistently supported by micromagnetic simulations. These results highlight the versatility of topological spin textures in centrosymmetric uniaxial magnets, thereby paving the way for the development of room-temperature topological spintronic devices with multi-Q characteristics.

19.
Adv Mater ; 35(32): e2301339, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37308132

RESUMO

Heat current in ferromagnets can generate a transverse electric voltage perpendicular to magnetization, known as anomalous Nernst effect (ANE). ANE originates intrinsically from the combination of large Berry curvature and density of states near the Fermi energy. It shows technical advantages over the conventional longitudinal Seebeck effect in converting waste heat to electricity due to its unique transverse geometry. However, materials showing giant ANE remain to be explored. Herein,  a large ANE thermopower of Syx ≈ 2 µV K-1 at room temperature in ferromagnetic Fe3 Pt epitaxial films is reported, which also show a giant transverse thermoelectric conductivity of αyx ≈ 4 A K-1  m-1 and a remarkable coercive field of 1300 Oe. The theoretical analysis reveals that the strong spin-orbit interaction in addition to the hybridization between Pt 5d and Fe 3d electrons leads to a series of distinct energy gaps and large Berry curvature in the Brillouin zone, which is the key for the large ANE. These results highlight the important roles of both Berry curvature and spin-orbit coupling in achieving large ANE at zero magnetic field, providing pathways to explore materials with giant transverse thermoelectric effect without an external magnetic field.

20.
Nano Lett ; 23(14): 6449-6457, 2023 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-37379096

RESUMO

Spin obit torque (SOT) driven magnetization switching has been used widely for encoding consumption-efficient memory and logic. However, symmetry breaking under a magnetic field is required to realize the deterministic switching in synthetic antiferromagnets with perpendicular magnetic anisotropy (PMA), which limits their potential applications. Herein, we report all electric-controlled magnetization switching in the antiferromagnetic Co/Ir/Co trilayers with vertical magnetic imbalance. Besides, the switching polarity could be reversed by optimizing the Ir thickness. By using the polarized neutron reflection (PNR) measurements, the canted noncollinear spin configuration was observed in Co/Ir/Co trilayers, which results from the competition of magnetic inhomogeneity. In addition, the asymmetric domain walls demonstrated by micromagnetic simulations result from introducing imbalance magnetism, leading to the deterministic magnetization switching in Co/Ir/Co trilayers. Our findings highlight a promising route to electric-controlled magnetism via tunable spin configuration, improve our understanding of physical mechanisms, and significantly promote industrial applications in spintronic devices.

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