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1.
ACS Omega ; 9(2): 2547-2558, 2024 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-38250393

RESUMO

To investigate the stability of nanobubbles in natural hard water, a series of eight samples ranging in hardness from 0 to 332 mg/L CaCO3 were sonicated for periods of 5-45 min with an ultrasonic horn. Conductivity, temperature, ζ-potential, composition, and pH of the water were analyzed, together with the crystal structure of any calcium carbonate precipitate. Quasi-stable populations of bulk nanobubbles in Millipore and soft water are characterized by a ζ-potential of -35 to -20 mV, decaying over 60 h or more. After sonicating the hardest waters for about 10 min, they turn cloudy due to precipitation of amorphous calcium carbonate when the water temperature reaches 40 °C; the ζ-potential then jumps from -10 to +20 mV and remains positive for several days. From an analysis of the change of conductivity of the hard water before and after sonication, it is estimated that 37 ± 5% of calcium was not originally in solution but existed in nanoscale prenucleation clusters, which decorate the nanobubbles formed in the early stages of sonication. Heating and charge screening in the nanobubble colloid cause the decorated bubbles to collapse or disperse, leaving an amorphous precursor of aragonite. Sonicating the soft supernatant increases its conductivity and pH and restores the negative ζ-potential associated with bulk nanobubbles, but there is no further precipitation. Our study of the correlation between nanobubble production and calcium agglomeration spanning the hardness and composition ranges of natural waters shows that the sonication method for introducing nanobubbles is viable only for hard water if it is kept cold; the stability of the nanobubble colloid will be reduced in any case by the presence of dissolved calcium and magnesium.

3.
Proc Natl Acad Sci U S A ; 120(36): e2302466120, 2023 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-37639599

RESUMO

The topological ferromagnet CoS2 exhibits an anhysteretic, weakly first-order transition at the Curie temperature of 119.8 K with a tricritical point µ0Htcp at 0.034 T. Magnetic symmetry and the mixing of majority and minority spin eg bands at a subband crossing just above the Fermi level produce a topological component of the magnetization that leads to a negative M3 term in the Landau free energy. The position of the Fermi level relative to the subband crossing is critical for controlling the order of the transition. Hole doping in Co0.89Fe0.11S2 drains the minority-spin eg pocket and results in a normal second-order phase transition. Electron doping in Co0.94Ni0.06S2 raises the Fermi level toward the subband gap, producing a strongly first-order transition with 15 K hysteresis. Our results demonstrate a relation between topological electronic structure and thermal hysteresis at the Curie point, which may help in the search for magnetocaloric materials.

4.
J Colloid Interface Sci ; 629(Pt B): 814-824, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36195021

RESUMO

HYPOTHESIS: Ortho and para water are the two nuclear isomers where the hydrogen protons align to give a total nuclear spin of 1 or 0. The equilibrium ratio of 3:1 is established slowly in freshly evaporated water vapour while the isomers behave distinct gasses, with their own partial pressures. Magnetic-field-induced ortho âŸ· para transformations are expected to alter the evaporation rate. EXPERIMENT: Evaporation from beakers of deionized water and a 6 M solution of urea is monitored simultaneously for periods from 1 to 60 h with and without a 500 mT magnetic field, while logging the ambient temperature and humidity. Balances with the two beakers are shielded in the same Perspex container. Many runs have been conducted over a two-year period. FINDINGS: The evaporation rate of water is found to increase by 12 ± 7% of in the field but that of water with dissolved urea decreases by 28 ± 6%. Two effects are at play. One is dephasing of the Larmor precession of adjacent protons on a water molecule in a field gradient, which tends to equalize the isomer populations. The other is Lorentz stress on the moving charge dipole, which can increase the proportion of the ortho isomer. From analysis of the time and field dependence of the evaporation, we infer that the ortho fraction is 39 ± 1% in fresh vapour from water and 60 ± 5% in fresh vapour from urea.

5.
J Phys Condens Matter ; 35(5)2022 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-36384048

RESUMO

An overview of the effect of a magnetic field gradient on fluids with linear magnetic susceptibilities is given. It is shown that two commonly encountered expressions, the magnetic field gradient force and the concentration gradient force for paramagnetic species in solution are equivalent for incompressible fluids. The magnetic field gradient and concentration gradient forces are approximations of the Kelvin force and Korteweg-Helmholtz force densities, respectively. The criterion for the appearance of magnetically induced convection is derived. Experimental work in which magnetically induced convection plays a role is reviewed.

6.
J Phys Chem C Nanomater Interfaces ; 125(40): 21831-21839, 2021 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-34676016

RESUMO

The electrosorption of Gd3+ ions from an aqueous 70 mM Gd(NO3)3 solution in monolithic carbon aerogel electrodes was recorded by dynamic neutron imaging. The aerogels have a bimodal pore size distribution consisting of macropores and mesopores centered at 115 and 15 nm, respectively. After the uptake of Gd3+ ions by the negatively charged surface of the porous structure, an inhomogeneous magnetic field was applied to the system of discharging electrodes. This led to a convective flow and confinement of Gd(NO3)3 solution in the magnetic field gradient. Thus, a way to desalt and capture paramagnetic ions from an initially homogeneous solution is established.

7.
J Am Chem Soc ; 143(31): 11914-11918, 2021 08 11.
Artigo em Inglês | MEDLINE | ID: mdl-34342435

RESUMO

Controlling supramolecular polymerization is of fundamental importance to create advanced materials and devices. Here we show that the thermodynamic equilibrium of Gd3+-bearing supramolecular rod networks is shifted reversibly at room temperature in a static magnetic field of up to 2 T. Our approach opens opportunities to control the structure formation of other supramolecular or coordination polymers that contain paramagnetic ions.

8.
Phys Rev Lett ; 126(17): 177401, 2021 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-33988409

RESUMO

The connection between chirality and electromagnetism has attracted much attention through the recent history of science, allowing the discovery of crucial nonreciprocal optical phenomena within the context of fundamental interactions between matter and light. A major phenomenon within this family is the so-called Faraday chiral anisotropy, the long-predicted but yet unobserved effect which arises due to the correlated coaction of both natural and magnetically induced optical activities at concurring wavelengths in chiral systems. Here, we report on the detection of the elusive anisotropic Faraday chiral phenomenon and demonstrate its enantioselectivity. The existence of this fundamental effect reveals the accomplishment of envisioned nonreciprocal electromagnetic metamaterials referred to as Faraday chiral media, systems where novel electromagnetic phenomena such as negative refraction of light at tunable wavelengths or even negative reflection can be realized. From a more comprehensive perspective, our findings have profound implications for the general understanding of parity-violating photon-particle interactions in magnetized media.

9.
Phys Rev Lett ; 126(17): 177202, 2021 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-33988421

RESUMO

All-optical reswitching has been investigated in the half-metallic Heusler ferrimagnet Mn_{2}Ru_{0.9}Ga, where Mn atoms occupy two inequivalent sites in the XA-type structure. The effect of a second 200 fs, 800 nm laser pulse that follows the first pump pulse, when both are above the threshold for switching, is studied as a function of t_{12}, the time between them. Aims were to determine the minimum time needed for reswitching and to identify the physical mechanisms involved. The time trajectory of the switching process on a plot of sublattice angular momentum, S^{4a} vs S^{4c}, is in three stages; when t<0.1 ps, the sublattice moments are rapidly disordered, but not destroyed, while conserving net angular momentum via optical spin-wave excitations. This leads to transient parallel alignment of the residual Mn spins in the first quadrant. The net angular momentum associated with the majority sublattice then flips after about 2 ps, and a fully reversed ferrimagnetic state is then established via the spin-lattice interaction, which allows reswitching provided t_{12}>10 ps.

10.
Nat Commun ; 12(1): 1668, 2021 Mar 12.
Artigo em Inglês | MEDLINE | ID: mdl-33712582

RESUMO

Antiferromagnetic insulators are a ubiquitous class of magnetic materials, holding the promise of low-dissipation spin-based computing devices that can display ultra-fast switching and are robust against stray fields. However, their imperviousness to magnetic fields also makes them difficult to control in a reversible and scalable manner. Here we demonstrate a novel proof-of-principle ionic approach to control the spin reorientation (Morin) transition reversibly in the common antiferromagnetic insulator α-Fe2O3 (haematite) - now an emerging spintronic material that hosts topological antiferromagnetic spin-textures and long magnon-diffusion lengths. We use a low-temperature catalytic-spillover process involving the post-growth incorporation or removal of hydrogen from α-Fe2O3 thin films. Hydrogenation drives pronounced changes in its magnetic anisotropy, Néel vector orientation and canted magnetism via electron injection and local distortions. We explain these effects with a detailed magnetic anisotropy model and first-principles calculations. Tailoring our work for future applications, we demonstrate reversible control of the room-temperature spin-state by doping/expelling hydrogen in Rh-substituted α-Fe2O3.

11.
J Phys Condens Matter ; 33(13): 135804, 2021 Feb 02.
Artigo em Inglês | MEDLINE | ID: mdl-33527913

RESUMO

We study the demagnetization dynamics of the fully compensated half-metallic ferrimagnet Mn2Ru x Ga. While the two antiferromagnetically coupled sublattices are both composed of manganese, they exhibit different temperature dependencies due to their differing local environments. The sublattice magnetization dynamics triggered by femtosecond laser pulses are studied to reveal the roles played by the spin and intersublattice exchange. We find a two-step demagnetization process, similar to the well-established case of Gd(FeCo)3, where on a 5 ps timescale the two Mn-sublattices seem to have different demagnetization rates. The behaviour is analysed using a four-temperature model, assigning different temperatures to the two manganese spin baths. Even in this strongly exchange-coupled system, the two spin reservoirs have considerably different behaviour. The half-metallic nature and strong exchange coupling of Mn2Ru x Ga lead to spin angular momentum conservation at much shorter time scales than found for Gd(FeCo)3 which suggests that low-power, sub-picosecond switching of the net moment of Mn2Ru x Ga is possible.

12.
Nat Commun ; 11(1): 4444, 2020 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-32895392

RESUMO

Energy-efficient control of magnetization without the help of a magnetic field is a key goal of spintronics. Purely heat-induced single-pulse all-optical toggle switching has been demonstrated, but so far only in Gd-based amorphous ferrimagnet films. In this work, we demonstrate toggle switching in films of the half-metallic ferrimagnetic Heusler alloys Mn2RuxGa, which have two crystallographically-inequivalent Mn sublattices. Moreover, we observe the switching at room temperature in samples that are immune to external magnetic fields in excess of 1 T, provided they exhibit a compensation point above room temperature. Observation of the effect in compensated ferrimagnets without Gd challenges our understanding of all-optical switching. The dynamic behavior indicates that Mn2RuxGa switches in 2 ps or less. Our findings widen the basis for fast optical switching of magnetization and break new ground for engineered materials that can be used for nonvolatile ultrafast switches using ultrashort pulses of light.

13.
Nano Lett ; 20(10): 7036-7042, 2020 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-32931289

RESUMO

Spin orbit torque driven switching is a favorable way to manipulate nanoscale magnetic objects for both memory and wireless communication devices. The critical current required to switch from one magnetic state to another depends on the geometry and the intrinsic properties of the materials used, which are difficult to control locally. Here, we demonstrate how focused helium ion beam irradiation can modulate the local magnetic anisotropy of a Co thin film at the microscopic scale. Real-time in situ characterization using the anomalous Hall effect showed up to an order of magnitude reduction of the magnetic anisotropy under irradiation, with multilevel switching demonstrated. The result is that spin-switching current densities, down to 800 kA cm-2, can be achieved on predetermined areas of the film, without the need for lithography. The ability to vary critical currents spatially has implications not only for storage elements but also neuromorphic and probabilistic computing.

14.
Nature ; 581(7806): 58-62, 2020 05.
Artigo em Inglês | MEDLINE | ID: mdl-32376963

RESUMO

When miniaturizing fluidic circuitry, the solid walls of the fluid channels become increasingly important1 because they limit the flow rates achievable for a given pressure drop, and they are prone to fouling2. Approaches for reducing the wall interactions include hydrophobic coatings3, liquid-infused porous surfaces4-6, nanoparticle surfactant jamming7, changes to surface electronic structure8, electrowetting9,10, surface tension pinning11,12 and use of atomically flat channels13. A better solution may be to avoid the solid walls altogether. Droplet microfluidics and sheath flow achieve this but require continuous flow of the central liquid and the surrounding liquid1,14. Here we demonstrate an approach in which aqueous liquid channels are surrounded by an immiscible magnetic liquid, both of which are stabilized by a quadrupolar magnetic field. This creates self-healing, non-clogging, anti-fouling and near-frictionless liquid-in-liquid fluidic channels. Manipulation of the field provides flow control, such as valving, splitting, merging and pumping. The latter is achieved by moving permanent magnets that have no physical contact with the liquid channel. We show that this magnetostaltic pumping method can be used to transport whole human blood with very little damage due to shear forces. Haemolysis (rupture of blood cells) is reduced by an order of magnitude compared with traditional peristaltic pumping, in which blood is mechanically squeezed through a plastic tube. Our liquid-in-liquid approach provides new ways to transport delicate liquids, particularly when scaling channels down to the micrometre scale, with no need for high pressures, and could also be used for microfluidic circuitry.

15.
Nat Mater ; 18(7): 770, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31182780

RESUMO

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

16.
Nat Mater ; 18(7): 652-656, 2019 07.
Artigo em Inglês | MEDLINE | ID: mdl-31086319
17.
Phys Rev Lett ; 121(14): 146802, 2018 Oct 05.
Artigo em Inglês | MEDLINE | ID: mdl-30339445

RESUMO

Electrolyte gating is a powerful means for tuning the carrier density and exploring the resultant modulation of novel properties on solid surfaces. However, the mechanism, especially its effect on the oxygen migration and electrostatic charging at the oxide heterostructures, is still unclear. Here we explore the electrolyte gating on oxygen-deficient interfaces between SrTiO_{3} (STO) crystals and LaAlO_{3} (LAO) overlayer through the measurements of electrical transport, x-ray absorption spectroscopy, and photoluminescence spectra. We found that oxygen vacancies (O_{vac}) were filled selectively and irreversibly after gating due to oxygen electromigration at the amorphous LAO/STO interface, resulting in a reconstruction of its interfacial band structure. Because of the filling of O_{vac}, the amorphous interface also showed an enhanced electron mobility and quantum oscillation of the conductance. Further, the filling effect could be controlled by the degree of the crystallinity of the LAO overlayer by varying the growth temperatures. Our results reveal the different effects induced by electrolyte gating, providing further clues to understand the mechanism of electrolyte gating on buried interfaces and also opening a new avenue for constructing high-mobility oxide interfaces.

18.
Nat Commun ; 9(1): 1897, 2018 05 15.
Artigo em Inglês | MEDLINE | ID: mdl-29765044

RESUMO

Complex-oxide materials exhibit physical properties that involve the interplay of charge and spin degrees of freedom. However, an ambipolar oxide that is able to exhibit both electron-doped and hole-doped ferromagnetism in the same material has proved elusive. Here we report ambipolar ferromagnetism in LaMnO3, with electron-hole asymmetry of the ferromagnetic order. Starting from an undoped atomically thin LaMnO3 film, we electrostatically dope the material with electrons or holes according to the polarity of a voltage applied across an ionic liquid gate. Magnetotransport characterization reveals that an increase of either electron-doping or hole-doping induced ferromagnetic order in this antiferromagnetic compound, and leads to an insulator-to-metal transition with colossal magnetoresistance showing electron-hole asymmetry. These findings are supported by density functional theory calculations, showing that strengthening of the inter-plane ferromagnetic exchange interaction is the origin of the ambipolar ferromagnetism. The result raises the prospect of exploiting ambipolar magnetic functionality in strongly correlated electron systems.

19.
Nature ; 556(7699): E5-E7, 2018 04 04.
Artigo em Inglês | MEDLINE | ID: mdl-29620726
20.
ACS Appl Mater Interfaces ; 9(51): 44931-44937, 2017 Dec 27.
Artigo em Inglês | MEDLINE | ID: mdl-29236463

RESUMO

Engineering ferromagnetism, by modulating its magnitude or anisotropy, is an important topic in the field of magnetism and spintronics. Among different types of magnetic materials, ferromagnetic insulators, in which magnetic moment unusually coexists with localized electrons, are of particular interest. Here, we report a remarkable interfacial enhancement of the ferromagnetism by adding one unit-cell LaAlO3 adjacent to an insulating LaMnO3 ultrathin film. The enhancement of ferromagnetism is explained in terms of charge transfer at the interface, as evidenced by X-ray absorption spectroscopy and ab initio calculations. This study demonstrates an effective and dramatic approach to modulate the functionality of ferromagnetic insulators, contributing to the arsenal of engineering techniques for future spintronics.

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