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1.
Nat Commun ; 13(1): 2141, 2022 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-35440657

RESUMO

Intermetallic compounds containing f-electron elements have been prototypical materials for investigating strong electron correlations and quantum criticality (QC). Their heavy fermion ground state evoked by the magnetic f-electrons is susceptible to the onset of quantum phases, such as magnetism or superconductivity, due to the enhanced effective mass (m*) and a corresponding decrease of the Fermi temperature. However, the presence of f-electron valence fluctuations to a non-magnetic state is regarded an anathema to QC, as it usually generates a paramagnetic Fermi-liquid state with quasiparticles of moderate m*. Such systems are typically isotropic, with a characteristic energy scale T0 of the order of hundreds of kelvins that require large magnetic fields or pressures to promote a valence or magnetic instability. Here we show the discovery of a quantum critical behaviour and a Lifshitz transition under low magnetic field in an intermediate valence compound α-YbAlB4. The QC origin is attributed to the anisotropic hybridization between the conduction and localized f-electrons. These findings suggest a new route to bypass the large valence energy scale in developing the QC.

2.
Nat Commun ; 11(1): 3144, 2020 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-32561729

RESUMO

Since the discovery of the Verwey transition in magnetite, transition metal compounds with pyrochlore structures have been intensively studied as a platform for realizing remarkable electronic phase transitions. We report on a phase transition that preserves the cubic symmetry of the ß-pyrochlore oxide CsW2O6, where each of W 5d electrons are confined in regular-triangle W3 trimers. This trimer formation represents the self-organization of 5d electrons, which can be resolved into a charge order satisfying the Anderson condition in a nontrivial way, orbital order caused by the distortion of WO6 octahedra, and the formation of a spin-singlet pair in a regular-triangle trimer. An electronic instability due to the unusual three-dimensional nesting of Fermi surfaces and the strong correlations of the 5d electrons characteristic of the pyrochlore oxides are both likely to play important roles in this charge-orbital-spin coupled phenomenon.

3.
Phys Rev Lett ; 117(10): 107203, 2016 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-27636491

RESUMO

The effects of pressure on a quantum spin liquid are investigated in an organic Mott insulator κ-(ET)_{2}Ag_{2}(CN)_{3} with a spin-1/2 triangular lattice. The application of negative chemical pressure to κ-(ET)_{2}Cu_{2}(CN)_{3}, which is a well-known sister Mott insulator, allows for extensive tuning of antiferromagnetic exchange coupling, with J/k_{B}=175-310 K, under hydrostatic pressure. Based on ^{13}C nuclear magnetic resonance measurements under pressure, we uncover universal scaling in the static and dynamic spin susceptibilities down to low temperatures ∼0.1k_{B}T/J. The persistent fluctuations and residual specific heat coefficient are consistent with the presence of gapless low-lying excitations. Our results thus demonstrate the fundamental finite-temperature properties of a quantum spin liquid in a wide parameter range.

4.
ACS Appl Mater Interfaces ; 7(31): 17188-98, 2015 Aug 12.
Artigo em Inglês | MEDLINE | ID: mdl-26189509

RESUMO

The direct synthesis of the adhered Ni-Al LDH thin film onto the surface of electrically conductive substrates by the liquid phase deposition (LPD) reaction is carried out for the development of the positive electrode. The complexation and solution equilibria of the dissolved species in the LPD reaction have been clarified by a theoretical approach, and the LPD reaction conditions for the Ni-Al LDH depositions are shown to be optimized by controlling the fluoride ion concentration and the pH of the LPD reaction solutions. The yields of metal oxides and hydroxides by the LPD method are very sensitive to the supersaturation state of the hydroxide in the reaction solution. The surfaces of conductive substrates are completely covered by the minute mesh-like Ni-Al LDH thin film; furthermore, there is no gap between the surfaces of conductive substrates and the deposited Ni-Al LDH thin film. The active material layer thickness was able to be controlled within the range from 100 nm to 1 µm by the LPD reaction time. The high-crystallinity and the arbitrary-thickness thin films on the conductive substrate surface will be beneficial for the interface control of charge transfer reaction fields and the internal resistance reduction of various secondary batteries.

5.
Phys Rev Lett ; 113(22): 227204, 2014 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-25494086

RESUMO

We report ^{7}Li-NMR studies on LiInCr_{4}O_{8} and LiGaCr_{4}O_{8}, in which Cr^{3+} ions with spin 3/2 form a breathing pyrochlore lattice, a network of tetrahedra with alternating sizes. In LiInCr_{4}O_{8} with large alternation, the nuclear relaxation rate 1/T_{1} shows an activated temperature (T) dependence down to 18 K, indicating a singlet ground state with a spin gap. This behavior, however, is disrupted by an antiferromagnetic transition at 13 K, which is preceded by another, most likely structural, transition at 16 K. In contrast, LiGaCr_{4}O_{8} with a small alternation shows no spin gap but exhibits a first-order antiferromagnetic transition over a distributed T range 13-20 K. Nevertheless, 1/T_{1} of the paramagnetic phase diverges toward 13 K, indicating proximity to a second-order transition. The results indicate that LiGaCr_{4}O_{8} is located in the vicinity of a tricritical point in the phase diagram.

6.
Phys Rev Lett ; 101(8): 086404, 2008 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-18764646

RESUMO

We have synthesized a new spinel oxide LiRh2O4 with a mixed-valent configuration of Rh3+ and Rh4+. At room temperature, it is a paramagnetic metal, but on cooling, a metal-insulator transition occurs and a valence bond solid state is formed below 170 K. We argue that the formation of valence bond solid is promoted by a band Jahn-Teller transition at 230 K and the resultant confinement of t_{2g} holes within the xy band. The band Jahn-Teller instability is also responsible for the observed enhanced thermoelectric power in the orbital-disordered phase above 230 K.

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