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1.
Nat Phys ; 20(4): 579-584, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38638456

RESUMO

Spontaneously broken symmetries are at the heart of many phenomena of quantum matter and physics more generally. However, determining the exact symmetries that are broken can be challenging due to imperfections such as strain, in particular when multiple electronic orders are competing. This is exemplified by charge order in some kagome systems, where evidence of nematicity and flux order from orbital currents remains inconclusive due to contradictory measurements. Here we clarify this controversy by fabricating highly symmetric samples of a member of this family, CsV3Sb5, and measuring their transport properties. We find that a measurable anisotropy is absent at any temperature in the unperturbed material. However, a pronounced in-plane transport anisotropy appears when either weak magnetic fields or strains are present. A symmetry analysis indicates that a perpendicular magnetic field can indeed lead to in-plane anisotropy by inducing a flux order coexisting with more conventional bond order. Our results provide a unifying picture for the controversial charge order in kagome metals and highlight the need for materials control at the microscopic scale in the identification of broken symmetries.

2.
Adv Mater ; : e2312524, 2024 Mar 14.
Artigo em Inglês | MEDLINE | ID: mdl-38482969

RESUMO

Catalytic materials play crucial roles in various energy-related processes, ranging from large-scale chemical production to advancements in renewable energy technologies. Despite a century of dedicated research, major enduring challenges associated with enhancing catalyst efficiency and durability, particularly in green energy-related electrochemical reactions, remain. Focusing only on either the crystal structure or electronic structure of a catalyst is deemed insufficient to break the linear scaling relationship (LSR), which is the golden rule for the design of advanced catalysts. The discourse in this review intricately outlines the essence of heterogenous catalysis reactions by highlighting the vital roles played by electron properties. The physical and electrochemical properties of electron charge and spin that govern catalysis efficiencies are analyzed. Emphasis is placed on the pronounced influence of external fields in perturbing the LSR, underscoring the vital role that electron spin plays in advancing high-performance catalyst design. The review culminates by proffering insights into the potential applications of spin catalysis, concluding with a discussion of extant challenges and inherent limitations. This article is protected by copyright. All rights reserved.

3.
Nat Commun ; 15(1): 1467, 2024 Feb 17.
Artigo em Inglês | MEDLINE | ID: mdl-38368411

RESUMO

The noncentrosymmetric ferromagnetic Weyl semimetal CeAlSi with simultaneous space-inversion and time-reversal symmetry breaking provides a unique platform for exploring novel topological states. Here, by employing multiple experimental techniques, we demonstrate that ferromagnetism and pressure can serve as efficient parameters to tune the positions of Weyl nodes in CeAlSi. At ambient pressure, a magnetism-facilitated anomalous Hall/Nernst effect (AHE/ANE) is uncovered. Angle-resolved photoemission spectroscopy (ARPES) measurements demonstrated that the Weyl nodes with opposite chirality are moving away from each other upon entering the ferromagnetic phase. Under pressure, by tracing the pressure evolution of AHE and band structure, we demonstrate that pressure could also serve as a pivotal knob to tune the positions of Weyl nodes. Moreover, multiple pressure-induced phase transitions are also revealed. These findings indicate that CeAlSi provides a unique and tunable platform for exploring exotic topological physics and electron correlations, as well as catering to potential applications, such as spintronics.

4.
Nat Commun ; 15(1): 710, 2024 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-38267457

RESUMO

Semiconductor transistors operate by modulating the charge carrier concentration of a channel material through an electric field coupled by a capacitor. This mechanism is constrained by the fundamental transport physics and material properties of such devices-attenuation of the electric field, and limited mobility and charge carrier density in semiconductor channels. In this work, we demonstrate a new type of transistor that operates through a different mechanism. The channel material is a Weyl semimetal, NbP, whose resistivity is modulated via a magnetic field generated by an integrated superconductor. Due to the exceptionally large electron mobility of this material, which reaches over 1,000,000 cm2/Vs, and the strong magnetoresistive coupling, the transistor can generate significant transconductance amplification at nanowatt levels of power. This type of device can enable new low-power amplifiers, suitable for qubit readout operation in quantum computers.

5.
Adv Mater ; 36(2): e2308151, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37853575

RESUMO

The exploration of quantum materials in which an applied thermo/electrical/magnetic field along one crystallographic direction produces an anisotropic response has led to unique functionalities. Along these lines, KMgBi is a layered, narrow gap semiconductor near a critical state between multiple Dirac phases due to the presence of a flat band near the Fermi level. The valence band is highly anisotropic with minimal cross-plane dispersion, which, in combination with an isotropic conduction band, enables axis-dependent conduction polarity. Thermopower and Hall measurements indicate dominant p-type conduction along the cross-plane direction, and n-type conduction along the in-plane direction, leading to a significant zero-field transverse thermoelectric response when the heat flux is at an angle to the principal crystallographic directions. Additionally, a large Ordinary Nernst effect (ONE) is observed with an applied field.  It arises from the ambipolar term in the Nernst effect, whereby the Lorentz force on electrons and holes makes them drift in opposite directions so that the resulting Nernst voltage becomes a function of the difference between their partial thermopowers, greatly enhancing the ONE. It is proven that axis-dependent polarity can synergistically enhance the ONE, in addition to leading to a zero-field transverse thermoelectric performance.

6.
Adv Mater ; 36(13): e2308746, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38126622

RESUMO

Chirality is a fundamental property of nature with relevance in biochemistry and physics, particularly in the field of catalysis. Understanding the mechanisms underlying chirality transfer is crucial for advancing the knowledge of chiral-related catalysis. Chiral quantum materials with intriguing chirality-dependent electronic properties, such as spin-orbital coupling (SOC) and exotic spin/orbital angular momentum (SAM/OAM), open novel avenues for linking solid-state topologies with chiral catalysis. In this review, the growth of topological homochiral crystals (THCs) is described, and their applications in heterogeneous catalysis, including hydrogen evolution reaction (HER), oxygen electrocatalysis, and asymmetric catalysis are summarized. A possible link between chirality-dependent electronic properties and heterogeneous catalysis is discussed. Finally, existing challenges in this field are highlighted, and a brief outlook on the impact of THCs on the overarching chemical-physical research is presented.

7.
Sci Adv ; 9(45): eadi1428, 2023 Nov 10.
Artigo em Inglês | MEDLINE | ID: mdl-37948525

RESUMO

The direct manipulation of spins via light may provide a path toward ultrafast energy-efficient devices. However, distinguishing the microscopic processes that can occur during ultrafast laser excitation in magnetic alloys is challenging. Here, we study the Heusler compound Co2MnGa, a material that exhibits very strong light-induced spin transfers across the entire M-edge. By combining the element specificity of extreme ultraviolet high-harmonic probes with time-dependent density functional theory, we disentangle the competition between three ultrafast light-induced processes that occur in Co2MnGa: same-site Co-Co spin transfer, intersite Co-Mn spin transfer, and ultrafast spin flips mediated by spin-orbit coupling. By measuring the dynamic magnetic asymmetry across the entire M-edges of the two magnetic sublattices involved, we uncover the relative dominance of these processes at different probe energy regions and times during the laser pulse. Our combined approach enables a comprehensive microscopic interpretation of laser-induced magnetization dynamics on time scales shorter than 100 femtoseconds.

8.
Proc Natl Acad Sci U S A ; 120(48): e2305541120, 2023 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-37983495

RESUMO

The interplay between chirality and topology nurtures many exotic electronic properties. For instance, topological chiral semimetals display multifold chiral fermions that manifest nontrivial topological charge and spin texture. They are an ideal playground for exploring chirality-driven exotic physical phenomena. In this work, we reveal a monopole-like orbital-momentum locking texture on the three-dimensional Fermi surfaces of topological chiral semimetals with B20 structures (e.g., RhSi and PdGa). This orbital texture enables a large orbital Hall effect (OHE) and a giant orbital magnetoelectric (OME) effect in the presence of current flow. Different enantiomers exhibit the same OHE which can be converted to the spin Hall effect by spin-orbit coupling in materials. In contrast, the OME effect is chirality-dependent and much larger than its spin counterpart. Our work reveals the crucial role of orbital texture for understanding OHE and OME effects in topological chiral semimetals and paves the path for applications in orbitronics, spintronics, and enantiomer recognition.

9.
Nat Commun ; 14(1): 6583, 2023 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-37852969

RESUMO

Weyl semimetals exhibit exotic magnetotransport phenomena such as the chiral anomaly and surface-to-bulk quantum oscillations (Weyl orbits) due to chiral bulk states and topologically protected surface states. Here we report a unique transport property in crystals of the ferromagnetic nodal-line Weyl semimetal Co2MnGa that have been polished to micron thicknesses using a focused ion beam. These thin crystals exhibit a large planar resistance anisotropy (10 × ) with axes that rotate by 90 degrees between opposite faces of the crystal. We use symmetry arguments and electrostatic simulations to show that the observed anisotropy resembles that of an isotropic conductor with surface states that are impeded from hybridization with bulk states. The origin of these states awaits further experiments that can correlate the surface bands with the observed 90° twist.

10.
Phys Rev Lett ; 131(1): 016901, 2023 Jul 07.
Artigo em Inglês | MEDLINE | ID: mdl-37478434

RESUMO

We report high resolution polar Kerr effect measurements on CsV_{3}Sb_{5} single crystals in search of signatures of spontaneous time-reversal symmetry breaking below the charge-order transition at T^{*}≈94 K. Utilizing two different versions of zero-area loop Sagnac interferometers operating at 1550 nm wavelength, each with the fundamental attribute that without a time-reversal symmetry breaking sample at its path, the interferometer is perfectly reciprocal, we find no observable Kerr effect to within the noise floor limit of the apparatus at 30 nanoradians. Simultaneous coherent reflection ratio measurements confirm the sharpness of the charge-order transition in the same optical volume as the Kerr measurements. At finite magnetic field we observe a sharp onset of a diamagnetic shift in the Kerr signal at T^{*}, which persists down to the lowest temperature without change in trend. Since 1550 nm is an energy that was shown to capture all features of the optical properties of the material that interact with the charge-order transition, we are led to conclude that it is highly unlikely that time-reversal symmetry is broken in the charge ordered state in CsV_{3}Sb_{5}.

11.
J Am Chem Soc ; 145(23): 12920-12927, 2023 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-37267070

RESUMO

Magnetic interactions in combination with nontrivial band structures can give rise to several exotic physical properties such as a large anomalous Hall effect, the anomalous Nernst effect, and the topological Hall effect (THE). Antiferromagnetic (AFM) materials exhibit the THE due to the presence of nontrivial spin structures. EuCuAs crystallizes in a hexagonal structure with an AFM ground state (Néel temperature ∼ 16 K). In this work, we observe a large topological Hall resistivity of ∼7.4 µΩ-cm at 13 K which is significantly higher than the giant topological Hall effect of Gd2PdSi3 (∼3 µΩ-cm). Neutron diffraction experiments reveal that the spins form a transverse conical structure during the metamagnetic transition, resulting in the large THE. In addition, by controlling the magnetic ordering structure of EuCuAs with an external magnetic field, several fascinating topological states such as Dirac and Weyl semimetals have been revealed. These results suggest the possibility of spintronic devices based on antiferromagnets with tailored noncoplanar spin configurations.

12.
Angew Chem Int Ed Engl ; 62(27): e202303296, 2023 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-37113018

RESUMO

The study of heterogeneous reactions for enantiomeric processes based on inorganic crystals has been resurgent in recent years. However, the question remains how homochirality develops in nature and chemical reactions. Here, the successful growth of B20 group PdGa single crystals with different chiral lattices enabled us to achieve enantioselective recognition of 3,4-dihydroxyphenylalanine (DOPA) based on a new mechanism, namely orbital angular momentum (OAM) polarization. The orbital textures of PdGa crystals indicate large OAM polarization near the Fermi level and carrying opposite signs. A positive or negative magnetization in the [111] direction is expected depending on the chiral lattice of PdGa crystals. Due to this, the adsorption energies of PdGa crystals and DOPA molecules differ depending on how well the O-2p orbital of DOPA pairs with the Pd-4d orbital of PdGa. The results provide one possible explanation for how chirality arises in nature by providing an enantioselective route with pure inorganic crystals.

14.
Adv Mater ; 35(13): e2208965, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36745845

RESUMO

The increasing resistance of copper (Cu) interconnects for decreasing dimensions is a major challenge in continued downscaling of integrated circuits beyond the 7 nm technology node as it leads to unacceptable signal delays and power consumption in computing. The resistivity of Cu increases due to electron scattering at surfaces and grain boundaries at the nanoscale. Topological semimetals, owing to their topologically protected surface states and suppressed electron backscattering, are promising candidates to potentially replace current Cu interconnects. Here, we report the unprecedented resistivity scaling of topological metal molybdenum phosphide (MoP) nanowires, and it is shown that the resistivity values are superior to those of nanoscale Cu interconnects <500 nm2 cross-section areas. The cohesive energy of MoP suggests better stability against electromigration, enabling a barrier-free design . MoP nanowires are more resistant to surface oxidation than the 20 nm thick Cu. The thermal conductivity of MoP is comparable to those of Ru and Co. Most importantly, it is demonstrated that the dimensional scaling of MoP, in terms of line resistance versus total cross-sectional area, is competitive to those of effective Cu with barrier/liner and barrier-less Ru, suggesting MoP is an attractive alternative for the scaling challenge of Cu interconnects.

15.
Adv Sci (Weinh) ; 10(13): e2207121, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36828783

RESUMO

Weyl semimetal is a unique topological phase with topologically protected band crossings in the bulk and robust surface states called Fermi arcs. Weyl nodes always appear in pairs with opposite chiralities, and they need to have either time-reversal or inversion symmetry broken. When the time-reversal symmetry is broken the minimum number of Weyl points (WPs) is two. If these WPs are located at the Fermi level, they form an ideal Weyl semimetal (WSM). In this study, intrinsic ferromagnetic (FM) EuCd2 As2 are grown, predicted to be an ideal WSM and studied its electronic structure by angle-resolved photoemission spectroscopy, and scanning tunneling microscopy which agrees closely with the first principles calculations. Moreover, anomalous Hall conductivity and Nernst effect are observed, resulting from the non-zero Berry curvature, and the topological Hall effect arising from changes in the band structure caused by spin canting produced by magnetic fields. These findings can help realize several exotic quantum phenomena in inorganic topological materials that are otherwise difficult to assess because of the presence of multiple pairs of Weyl nodes.

16.
Phys Rev Lett ; 130(6): 066402, 2023 Feb 10.
Artigo em Inglês | MEDLINE | ID: mdl-36827563

RESUMO

Novel topological phases of matter are fruitful platforms for the discovery of unconventional electromagnetic phenomena. Higher-fold topology is one example, where the low-energy description goes beyond standard model analogs. Despite intensive experimental studies, conclusive evidence remains elusive for the multigap topological nature of higher-fold chiral fermions. In this Letter, we leverage a combination of fine-tuned chemical engineering and photoemission spectroscopy with photon energy contrast to discover the higher-fold topology of a chiral crystal. We identify all bulk branches of a higher-fold chiral fermion for the first time, critically important for allowing us to explore unique Fermi arc surface states in multiple interband gaps, which exhibit an emergent ladder structure. Through designer chemical gating of the samples in combination with our measurements, we uncover an unprecedented multigap bulk boundary correspondence. Our demonstration of multigap electronic topology will propel future research on unconventional topological responses.

17.
J Am Chem Soc ; 145(8): 4527-4533, 2023 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-36789888

RESUMO

Electrons in solids often adopt complex patterns of chemical bonding driven by the competition between energy gains from covalency and delocalization, and energy costs of double occupation to satisfy Pauli exclusion, with multiple intermediate states in the transition between highly localized, and magnetic, and delocalized, and nonmagnetic limits. Herein, we report a chemical pressure-driven transition from a proper Mn magnetic ordering phase transition to a Mn magnetic phase crossover in EuMn2P2 the limiting end member of the EuMn2X2 (X = Sb, As, P) family of layered materials. This loss of a magnetic ordering occurs despite EuMn2P2 remaining an insulator at all temperatures, and with a phase transition to long-range Eu antiferromagnetic order at TN ≈ 17 K. The absence of a Mn magnetic phase transition contrasts with the formation of long-range Mn order at T ≈ 130 K in isoelectronic EuMn2Sb2 and EuMn2As2. Temperature-dependent specific heat and 31P NMR measurements provide evidence for the development of short-range Mn magnetic correlations from T ≈ 250-100 K, interpreted as a precursor to covalent bond formation. Density functional theory calculations demonstrate an unusual sensitivity of the band structure to the details of the imposed Mn and Eu magnetic order, with an antiferromagnetic Mn arrangement required to recapitulate an insulating state. Our results imply a picture in which long-range Mn magnetic order is suppressed by chemical pressure, but that antiferromagnetic correlations persist, narrowing bands and producing an insulating state.

19.
Adv Mater ; 35(3): e2205927, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36385535

RESUMO

Kagome magnets provide a fascinating platform for a plethora of topological quantum phenomena, in which the delicate interplay between frustrated crystal structure, magnetization, and spin-orbit coupling (SOC) can engender highly tunable topological states. Here, utilizing angle-resolved photoemission spectroscopy, the Weyl lines are directly visualized with strong out-of-plane dispersion in the A-A stacked kagome magnet GdMn6 Sn6 . Remarkably, the Weyl lines exhibit a strong magnetization-direction-tunable SOC gap and binding energy tunability after substituting Gd with Tb and Li, respectively. These results not only illustrate the magnetization direction and valence counting as efficient tuning knobs for realizing and controlling distinct 3D topological phases, but also demonstrate AMn6 Sn6 (A = rare earth, or Li, Mg, or Ca) as a versatile material family for exploring diverse emergent topological quantum responses.

20.
Nat Commun ; 13(1): 7784, 2022 Dec 16.
Artigo em Inglês | MEDLINE | ID: mdl-36526636

RESUMO

Despite the fruitful achievements in the development of hydrogen production catalysts with record-breaking performances, there is still a lack of durable catalysts that could work under large current densities (>1000 mA cm-2). Here, we investigated the catalytic behaviors of Sr2RuO4 bulk single crystals. This crystal has demonstrated remarkable activities under the current density of 1000 mA cm-2, which require overpotentials of 182 and 278 mV in 0.5 M H2SO4 and 1 M KOH electrolytes, respectively. These materials are stable for 56 days of continuous testing at a high current density of above 1000 mA cm-2 and then under operating temperatures of 70 °C. The in-situ formation of ferromagnetic Ru clusters at the crystal surface is observed, endowing the single-crystal catalyst with low charge transfer resistance and high wettability for rapid gas bubble removal. These experiments exemplify the potential of designing HER catalysts that work under industrial-scale current density.

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