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1.
J Am Chem Soc ; 146(9): 5908-5915, 2024 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-38391353

RESUMO

Unconventional superconductivity in bulk materials under ambient pressure is extremely rare among the 3d transition metal compounds outside the layered cuprates and iron-based family. It is predominantly linked to highly anisotropic electronic properties and quasi-two-dimensional (2D) Fermi surfaces. To date, the only known example of a Co-based exotic superconductor is the hydrated layered cobaltate, NaxCoO2·yH2O, and its superconductivity is realized in the vicinity of a spin-1/2 Mott state. However, the nature of the superconductivity in these materials is still a subject of intense debate, and therefore, finding a new class of superconductors will help unravel the mysteries of their unconventional superconductivity. Here, we report the discovery of superconductivity at ∼6.3 K in our newly synthesized layered compound Na2CoSe2O, in which the edge-shared CoSe6 octahedra form [CoSe2] layers with a perfect triangular lattice of Co ions. It is the first 3d transition metal oxychalcogenide superconductor with distinct structural and chemical characteristics. Despite its relatively low TC, this material exhibits very high superconducting upper critical fields, µ0HC2(0), which far exceeds the Pauli paramagnetic limit by a factor of 3-4. First-principles calculations show that Na2CoSe2O is a rare example of a negative charge transfer superconductor. This cobalt oxychalcogenide with a geometrical frustration among Co spins shows great potential as a highly appealing candidate for the realization of unconventional and/or high-TC superconductivity beyond the well-established Cu- and Fe-based superconductor families and opens a new field in the physics and chemistry of low-dimensional superconductors.

2.
ACS Nano ; 18(28): 18327-18333, 2024 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-38958041

RESUMO

In van der Waals materials, external strain is an effective tool to manipulate and control electronic responses by changing the electronic bands upon lattice deformation. In particular, the band gap of the layered transition metal pentatelluride HfTe5 is sufficiently small to be inverted by subtle changes of the lattice parameters resulting in a strain-tunable topological phase transition. In that case, knowledge about the spatial homogeneity of electronic properties becomes crucial, especially for the microfabricated thin film circuits used in typical transport measurements. Here, we reveal the homogeneity of exfoliated HfTe5 thin films by spatially resolved Raman microscopy. Comparing the Raman spectra under applied external strain to unstrained bulk references, we pinpoint local variations of Raman signatures to inhomogeneous strain profiles in the sample. Importantly, our results demonstrate that microfabricated contacts can act as sources of significant inhomogeneities. To mitigate the impact of unintentional strain and its corresponding modifications of the electronic structure, careful Raman microscopy constitutes a valuable tool for quantifying the homogeneity of HfTe5 films and circuits fabricated thereof.

3.
PNAS Nexus ; 2(6): pgad164, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37266397

RESUMO

Iron-based superconductors provide a rich platform to investigate the interplay between unconventional superconductivity, nematicity, and magnetism. The electronic structure and the magnetic properties of iron-based superconductors are highly sensitive to the pnictogen height. Coherent excitation of the A1g phonon by femtosecond laser directly modulates the pnictogen height, which has been used to control the physical properties of iron-based superconductors. Previous studies show that the driven A1g phonon resulted in a transient increase of the pnictogen height in BaFe2As2, favoring an enhanced Fe magnetic moment. However, there are no direct observations on either the enhanced Fe magnetic moments or the enhanced spin-density wave (SDW) gap. Here, we use time-resolved broadband terahertz spectroscopy to investigate the dynamics of BaFe2As2 in the A1g phonon-driven state. Below the SDW transition temperature, we observe a transient gap generation at early-time delays. A similar transient feature is observed in the normal state up to room temperature.

4.
Sci Bull (Beijing) ; 68(9): 920-927, 2023 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-37085398

RESUMO

Pursuing efficient thermoelectricity from low-dimensional materials has been highly motivated since the seminal work of Hicks and Dresselhaus. In fact, many superior thermoelectric materials like Bi2Te3, Mg3Sb2/Mg3Bi2 and SnSe are quasi-two-dimensional (q2D), though the advantages of two-dimensionality appear to be diverse and sometimes controversial. Here, we report on a remarkably high thermoelectric performance in TlCu3Te2, which is quasi-one-dimensional (q1D) with a further reduced dimension. The thermoelectric figure of merit zT along its q1D axis amounts to 1.3 (1.5) at 300 (400) K, rivaling the best ever reported at these temperatures. The high thermoelectric performances benefit from, on one hand, large power factors derived from a center-hollowed, pancake-like Fermi pocket with q1D dispersion at the edge of a narrow band gap, and on the other hand, small lattice thermal conductivities caused by the large and anharmonic q1D lattice consisting of heavy, lone-pair-electron bearing (Tl+) and weakly-bonded (Cu+) ions. This compound represents the first bulk material with quasi-uniaxial thermoelectric transport of application level, offering a renewed opportunity to exploit reduced dimensionality for high-performance thermoelectricity.

5.
Chem Commun (Camb) ; 56(33): 4603-4606, 2020 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-32211653

RESUMO

Using 2% percent of iron dopants as reaction active sites yields a series of single crystals of 1,10-phenanthroline intercalated NiPS3, via a solution reaction with aniline chloride, not possible by a direct reaction. Experimental magnetic susceptibility measurements demonstrate that 1,10-phenanthroline intercalation suppresses the anti-ferromagnetism ordering at around 150 K in Fe0.02Ni0.98PS3, and gives rise to a ferrimagnetic phase transition at a temperature around 75 K. An intercalation mechanism is proposed for the reaction, and this dopant seeding method provides a new approach for intercalation into layered materials.

6.
Adv Mater ; 32(16): e1907970, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-32108388

RESUMO

Interfaces between materials with different electronic ground states have become powerful platforms for creating and controlling novel quantum states of matter, in which inversion symmetry breaking and other effects at the interface may introduce additional electronic states. Among the emergent phenomena, superconductivity is of particular interest. Here, by depositing metal films on a newly identified topological semimetal tungsten carbide (WC) single crystal, interfacial superconductivity is obtained, evidenced from soft point-contact spectroscopy. This very robust phenomenon is demonstrated for a wide range of metal/WC interfaces, involving both nonmagnetic and ferromagnetic films, and the superconducting transition temperatures are surprisingly insensitive to the magnetism of thin films. This method offers an opportunity to explore the long-sought topological superconductivity and has potential applications in topological-state-based spin devices.

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