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1.
Sci Technol Adv Mater ; 23(1): 858-865, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-36518983

RESUMEN

The thermal conductivity above room temperature is investigated for LaCoO3-based materials showing spin-state and insulator-metal crossovers. A positive temperature coefficient (PTC) of the thermal conductivity is observed during the insulator-metal crossover around 500 K. Our analysis indicates that the phononic thermal transport is also enhanced in addition to the electronic contribution as the insulator-metal crossover takes place. The enhancement of the phononic component is ascribed to the reduction of the incoherent local lattice distortion coupled with the spin/orbital state of each Co3+ ion, which is induced by the enhanced spin-state fluctuation between low and excited spin-states. Moreover, fine tunability for the PTC of the thermal conductivity is demonstrated via doping hole-type carriers into LaCoO3. The observed enhancement ratio of the thermal conductivity κ T (773 K) / κ T (323 K) = 2.6 in La0.95Sr0.05CoO3 is the largest value among oxide materials which exhibit a PTC of their thermal conductivity above room temperature. The thermal rectification ratio is estimated to reach 61% for a hypothetical thermal diode consisting of La0.95Sr0.05CoO3 and LaGaO3, the latter of which is a typical band insulator. These results indicate that utilizing spin-state and orbital degrees of freedom in strongly correlated materials is a useful strategy for tuning thermal transport properties, especially for designing thermal diodes.

2.
Proc Natl Acad Sci U S A ; 119(41): e2200958119, 2022 Oct 11.
Artículo en Inglés | MEDLINE | ID: mdl-36191237

RESUMEN

The manipulation and control of electron spins, the fundamental building blocks of magnetic domains and spin textures, are at the core of spintronics. Of particular interest is the effect of the electric current on topological magnetic skyrmions, such as the current-induced deformation of isolated skyrmions. The deformation has consequences ranging from perturbed dynamics to modified packing configurations. In this study, we measured the current-driven real-space deformation of isolated, pinned skyrmions within Co10Zn10 at room temperature. We observed that the skyrmions are surprisingly soft, readily deforming during electric current application into an elliptical shape with a well-defined deformation axis (semimajor axis). We found that this axis rotates unidirectionally toward the current direction irrespective of electric current polarity and that the elliptical deformation reverses back upon current termination. We quantified the average distortion δ, which increased by ∼90% during the largest applied current density |j| = 8.46 ×109 A/m2 when compared with the skyrmion's intrinsic shape ([Formula: see text]). Additionally, we demonstrated an approximately 120% average skyrmion core size expansion during current application, highlighting the skyrmions' inherent topological protection. This evaluation of in situ electric current-induced skyrmion deformation paints a clearer picture of spin-polarized electron-skyrmion interactions and may prove essential in designing spintronic devices.

3.
J Am Chem Soc ; 144(37): 16866-16871, 2022 Sep 21.
Artículo en Inglés | MEDLINE | ID: mdl-36066406

RESUMEN

Configurational entropy can impact crystallization processes, tipping the scales between structures of nearly equal internal energy. Using alloyed single crystals of Gd2PdSi3 in the AlB2-type structure, we explore the formation of complex layer sequences made from alternating, two-dimensional triangular and honeycomb slabs. A four-period and an eight-period stacking sequence are found to be very close in internal energy, the latter being favored by entropy associated with covering the full configuration space of interlayer bonds. Possible consequences of polytype formation on magnetism in Gd2PdSi3 are discussed.

4.
Proc Natl Acad Sci U S A ; 118(33)2021 Aug 17.
Artículo en Inglés | MEDLINE | ID: mdl-34389668

RESUMEN

The long-range order of noncoplanar magnetic textures with scalar spin chirality (SSC) can couple to conduction electrons to produce an additional (termed geometrical or topological) Hall effect. One such example is the Hall effect in the skyrmion lattice state with quantized SSC. An alternative route to attain a finite SSC is via the spin canting caused by thermal fluctuations in the vicinity of the ferromagnetic ordering transition. Here, we report that for a highly conducting ferromagnet with a two-dimensional array of spin trimers, the thermally generated SSC can give rise to a gigantic geometrical Hall conductivity even larger than the intrinsic anomalous Hall conductivity of the ground state. We also demonstrate that the SSC induced by thermal fluctuations leads to a strong response in the Nernst effect. A comparison of the sign and magnitude of fluctuation-Nernst and Hall responses in fundamental units indicates the need for a momentum-space picture to model these thermally induced signals.

5.
Phys Rev Lett ; 125(7): 076602, 2020 Aug 14.
Artículo en Inglés | MEDLINE | ID: mdl-32857583

RESUMEN

The topological Hall effect (THE) and its thermoelectric counterpart, the topological Nernst effect (TNE), are hallmarks of the skyrmion lattice phase (SkL). We observed the giant TNE of the SkL in centrosymmetric Gd_{2}PdSi_{3}, comparable in magnitude to the largest anomalous Nernst signals in ferromagnets. Significant enhancement (suppression) of the THE occurs when doping electrons (holes) to Gd_{2}PdSi_{3}. On the electron-doped side, the topological Hall conductivity approaches the characteristic threshold ∼1000 (Ω cm)^{-1} for the intrinsic regime. We use the filling-controlled samples to confirm Mott's relation between TNE and THE and discuss the importance of Gd-5d orbitals for transport in this compound.

6.
Nat Commun ; 10(1): 5831, 2019 12 24.
Artículo en Inglés | MEDLINE | ID: mdl-31874953

RESUMEN

Magnetic skyrmion textures are realized mainly in non-centrosymmetric, e.g. chiral or polar, magnets. Extending the field to centrosymmetric bulk materials is a rewarding challenge, where the released helicity/vorticity degree of freedom and higher skyrmion density result in intriguing new properties and enhanced functionality. We report here on the experimental observation of a skyrmion lattice (SkL) phase with large topological Hall effect and an incommensurate helical pitch as small as 2.8 nm in metallic Gd3Ru4Al12, which materializes a breathing kagomé lattice of Gadolinium moments. The magnetic structure of several ordered phases, including the SkL, is determined by resonant x-ray diffraction as well as small angle neutron scattering. The SkL and helical phases are also observed directly using Lorentz-transmission electron microscopy. Among several competing phases, the SkL is promoted over a low-temperature transverse conical state by thermal fluctuations in an intermediate range of magnetic fields.

7.
Science ; 365(6456): 914-918, 2019 08 30.
Artículo en Inglés | MEDLINE | ID: mdl-31395744

RESUMEN

Geometrically frustrated magnets can host complex spin textures, leading to unconventional electromagnetic responses. Magnetic frustration may also promote topologically nontrivial spin states such as magnetic skyrmions. Experimentally, however, skyrmions have largely been observed in noncentrosymmetric lattice structures or interfacial symmetry-breaking heterostructures. Here, we report the emergence of a Bloch-type skyrmion state in the frustrated centrosymmetric triangular-lattice magnet Gd2PdSi3 We observed a giant topological Hall response, indicating a field-induced skyrmion phase, which is further corroborated by the observation of in-plane spin modulation probed by resonant x-ray scattering. Our results may lead to further discoveries of emergent electrodynamics in magnetically frustrated centrosymmetric materials.

8.
J Am Chem Soc ; 140(48): 16396-16401, 2018 Dec 05.
Artículo en Inglés | MEDLINE | ID: mdl-30444605

RESUMEN

Optical properties of aqueous colloidal dispersions of 2D electrolytes, if their aspect ratios are extra-large, can be determined by their orientation preferences. Recently, we reported that a colloidal dispersion of diamagnetic titanate(IV) nanosheets (TiIVNSs), when placed in a magnetic field, is highly anisotropic because TiIVNS anomalously orients its 2D plane orthogonal to the magnetic flux lines due to its large anisotropic magnetic susceptibility. Herein, we report a serendipitous finding that TiIVNSs can be in situ photochemically reduced into a paramagnetic species (TiIV/IIINSs), so that their preference of magnetic orientation changes from orthogonal to parallel. This transition distinctly alters the structural anisotropy and therefore optical appearance of the colloidal dispersion in a magnetic field. We also found that TiIV/IIINSs is autoxidized back to TiIVNSs under non-deaerated conditions. By using an elaborate setup, the dispersion of TiIVNSs serves as an optical switch remotely operable by magnet and light.

9.
Sci Adv ; 4(9): eaar7043, 2018 09.
Artículo en Inglés | MEDLINE | ID: mdl-30225364

RESUMEN

Magnetic skyrmions are vortex-like topological spin textures often observed to form a triangular-lattice skyrmion crystal in structurally chiral magnets with the Dzyaloshinskii-Moriya interaction. Recently, ß-Mn structure-type Co-Zn-Mn alloys were identified as a new class of chiral magnet to host such skyrmion crystal phases, while ß-Mn itself is known as hosting an elemental geometrically frustrated spin liquid. We report the intermediate composition system Co7Zn7Mn6 to be a unique host of two disconnected, thermal-equilibrium topological skyrmion phases; one is a conventional skyrmion crystal phase stabilized by thermal fluctuations and restricted to exist just below the magnetic transition temperature Tc, and the other is a novel three-dimensionally disordered skyrmion phase that is stable well below Tc. The stability of this new disordered skyrmion phase is due to a cooperative interplay between the chiral magnetism with the Dzyaloshinskii-Moriya interaction and the frustrated magnetism inherent to ß-Mn.

10.
Sci Adv ; 4(8): eaat1115, 2018 08.
Artículo en Inglés | MEDLINE | ID: mdl-30105304

RESUMEN

Dynamics of string-like objects is an important issue in a broad range of physical systems, including vortex lines in superconductors, viscoelastic polymers, and superstrings in elementary particle physics. In noncentrosymmetric magnets, string forms of magnetic skyrmions are present as topological spin objects, and their current-induced dynamics has recently attracted intense interest. We show in the chiral magnet MnSi that the current-induced deformation dynamics of skyrmion strings results in transport response associated with the real-space Berry phase. Prominent nonlinear Hall signals emerge above the threshold current only in the skyrmion phase. We clarify the mechanism for these nonlinear Hall signals by adopting spin density wave picture to describe the moving skyrmion lattice; deformation of skyrmion strings occurs in an asymmetric manner due to the Dzyaloshinskii-Moriya interaction, which leads to the nonreciprocal nonlinear Hall response originating from an emergent electromagnetic field. This finding reveals the dynamical nature of string-like objects and consequent transport outcomes in noncentrosymmetric systems.

11.
Nat Commun ; 8(1): 1332, 2017 11 06.
Artículo en Inglés | MEDLINE | ID: mdl-29109474

RESUMEN

In the MnSi bulk chiral magnet, magnetic skyrmion strings of 17 nm in diameter appear in the form of a lattice, penetrating the sample thickness, 10-1000 µm. Although such a bundle of skyrmion strings may exhibit complex soft-matter-like dynamics when starting to move under the influence of a random pinning potential, the details remain highly elusive. Here, we show that a metastable skyrmion-string lattice is subject to topological unwinding under the application of pulsed currents of 3-5 × 106 A m-2 rather than being transported, as evidenced by measurements of the topological Hall effect. The critical current density above which the topological unwinding occurs is larger for a shorter pulse width, reminiscent of the viscoelastic characteristics accompanying the pinning-creep transition observed in domain-wall motion. Numerical simulations reveal that current-induced depinning of already segmented skyrmion strings initiates the topological unwinding. Thus, the skyrmion-string length is an element to consider when studying current-induced motion.

12.
Sci Adv ; 3(6): e1602562, 2017 06.
Artículo en Inglés | MEDLINE | ID: mdl-28630906

RESUMEN

Magnetic skyrmions exhibit particle-like properties owing to the topology of their swirling spin texture, providing opportunities to study crystallization of topological particles. However, they mostly end up with a triangular lattice, and thus, the packing degree of freedom in the skyrmion particles has been overlooked so far. We report a structural transition of the skyrmion lattice in MnSi. By use of small-angle neutron scattering, we explore a metastable skyrmion state spreading over a wide temperature and magnetic field region, after thermal quenching. The quenched skyrmions undergo a triangular-to-square lattice transition with decreasing magnetic field at low temperatures. Our study suggests that various skyrmion lattices can emerge at low temperatures, where the skyrmions exhibit distinct topological nature and high sensitivity to the local magnetic anisotropy arising from the underlying chemical lattice.

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