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Recently, considerable efforts have been made on research and improvement for Ni-rich lithium-ion batteries to meet the demand from vehicles and grid-level large-scale energy storage. Development of next-generation high-performance lithium-ion batteries requires a comprehensive understanding on the underlying electrochemical mechanisms associated with its structural evolution. In this work, advanced operando neutron diffraction and four-dimensional scanning transmission electron microscopy techniques are applied to clarify the structural evolution of electrodes in two distinct full cells with identical LiNi0.8Co0.1Mn0.1O2 cathode but different anode counterparts. It is found that both of cathodes in two cells exhibit non-intrinsic two-phase-like behavior at the early charge stage, indicating selective Li+ extraction from cathodes. But the heterogeneous evolution of cathode is less serious with graphite-silicon blended anode than that with graphite anode due to the different delithiation rate. Moreover, it is revealed that the formation of heterogeneous structure is led by the distribution of defects including Li/Ni disordering and microcracks, which should be inhibited by assembling appropriate anode to avoid potential threaten on cell performance. The present work unveils the origin of inhomogeneity in Ni-rich lithium-ion batteries and highlights the significance of kinetics control in electrodes for batteries with higher capacity and longer life., Comment: 29 pages and 5 figures for manuscript; 30 pages, 14 figures and 4 tables for supplementary information

We use neutron powder diffraction to investigate the magnetic and crystalline structure of Cr$_2$GaN. A magnetic phase transition is identified at $T \approx 170$ K, whereas no trace of structural transition is observed down to 6 K. Combining Rietveld refinement with irreducible representations, the spin configuration of Cr ions in Cr$_2$GaN is depicted as an incommensurate sinusoidal modulated structure characterized by a propagating vector ${k}$=(0.365, 0.365, 0). Upon warming up to the paramagnetic state, the magnetic order parameter closely resembles to the temperature dependence of $c$-axis lattice parameter, suggesting strong magneto-elastic coupling in this compound. Therefore, Cr$_2$GaN provides a potential platform for the exploration of magnetically tuned properties such as magnetoelectric, magnetostrictive and magnetocaloric effects, as well as their applications., Comment: 5 pages, 3 figures

The effects of Sr doping on the structural properties of Na$_{2}$BaCo(PO$_{4}$)$_{2}$, a spin-1/2 triangular-lattice antiferromagnet as a quantum spin liquid candidate, are investigated by complementary x-ray and neutron powder diffraction measurements. It is found that in Na$_{2}$Ba$_{1-x}$Sr$_{x}$Co(PO$_{4}$)$_{2}$ (NBSCPO), the trigonal phase (space group $\mathit{P}$$\bar{3}$$\mathit{m}$1) with a perfect triangular lattice of Co$^{2+}$ ions is structurally stable when the doping level of Sr is below 30% ($\mathit{x}$ $\le$ 0.3), while a pure monoclinic phase (space group $\mathit{P}$2$_{1}$/$\mathit{a}$) with slight rotations of CoO$_{6}$ octahedra and displacements of Ba$^{2+}$/Sr$^{2+}$ ions will be established when the Sr doping level is above 60% ($\mathit{x}$ $\ge$ 0.6). Such a doping-induced structural transformation in NBSCPO is supported by first-principles calculations and Raman spectroscopy. Na$_{2}$SrCo(PO$_{4}$)$_{2}$, a novel spin-1/2 triangular-lattice antiferromagnet with glaserite-type structure, although monoclinically distorted, exhibits no long-range magnetic order down to 2 K and a similar negative Curie-Weiss temperature as Na$_{2}$BaCo(PO$_{4}$)$_{2}$ with a perfect triangular lattice, suggesting the robustness of magnetic exchange interaction against the Ba/Sr substitutions., Comment: 26 pages, 7 figures

Small-angle neutron scattering (SANS) measurements are performed on the ferromagnetic superconductor EuFe$_{2}$(As$_{0.8}$P$_{0.2}$)$_{2}$ ($T\rm_{sc}=22.5\,$K) to probe the delicate interplay between ferromagnetism and superconductivity. A clear signature of large ferromagnetic domains is found below the ferromagnetic ordering temperature $T\rm_{C}$ = 18.5 K. In a small temperature interval of $\sim$ 1.5 K below $T\rm_{C}$, additional SANS signal is observed, of which the indirect Fourier transform reveals characteristic length scales in between $\sim$ 80 nm to $\sim$ 160 nm. These nanometer-scaled domain structures are identified to result from an intermediate inhomogeneous Meissner effect denoted domain Meissner state, which was recently observed on the surface of EuFe$_{2}$(As$_{0.79}$P$_{0.21}$)$_{2}$ crystals by means of magnetic force microscopy [V. S. Stolyarov $\mathit{et}$ $\mathit{al.}$, Sci. Adv. 4, 1061 (2018)], ascribing to the competition between ferromagnetism and superconductivity. Our measurements clearly render the domain Meissner state as a bulk phenomenon and provide a key solution to the mystery regarding the intriguing coexistence of strong ferromagnetism and bulk superconductivity in these compounds., Comment: 6 pages, 4 figures, accepted for publication in Physical Review B as a Letter

The ground-state magnetic structures of the Eu$^{2+}$ spins in recently discovered RbEu(Fe$_{1-x}$Ni$_{x}$)$_{4}$As$_{4}$ superconductors have been investigated by neutron powder diffraction measurements. It is found that as the superconductivity gets suppressed with the increase of Ni doping, the magnetic propagation vector of the Eu sublattice diminishes, corresponding to the decrease of the rotation angle between the moments in neighboring Eu layers. The ferromagnetic Eu layers are helically modulated along the $\mathit{c}$ axis with an incommensurate magnetic propagation vector in both the ferromagnetic superconductor RbEu(Fe$_{0.95}$Ni$_{0.05}$)$_{4}$As$_{4}$ and the superconducting ferromagnet RbEu(Fe$_{0.93}$Ni$_{0.07}$)$_{4}$As$_{4}$. Such a helical structure transforms into a purely collinear ferromagnetic structure for non-superconducting RbEu(Fe$_{0.91}$Ni$_{0.09}$)$_{4}$As$_{4}$, with all the Eu$^{2+}$ spins lying along the tetragonal (1 1 0) direction. The evolution from helical to collinear ferromagnetic order of the Eu$^{2+}$ spins with increasing Ni doping is supported by first-principles calculations. The variation of the rotation angle between adjacent Eu$^{2+}$ layers can be well explained by considering the change of magnetic exchange couplings mediated by the indirect Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction., Comment: 9 pages, 6 figures, accepted for publication in Physical Review Research

The crystalline structure, magnetism, and magnetocaloric effect of a GdCrO$_3$ single crystal grown with the laser-diode-heated floating-zone technique have been studied. The GdCrO$_3$ single crystal crystallizes into an orthorhombic structure with the space group $Pmnb$ at room temperature. Upon cooling, under a magnetic field of 0.1 T, it undergoes a magnetic phase transition at $T_{\textrm{N-Cr}} =$ 169.28(2) K with Cr$^{3+}$ ions forming a canted antiferromagnetic (AFM) structure, accompanied by a weak ferromagnetism. Subsequently, a spin reorientation takes place at $T_{\textrm{SR}} =$ 5.18(2) K due to Gd$^{3+}$-Cr$^{3+}$ magnetic couplings. Finally, the long-range AFM order of Gd$^{3+}$ ions establishes at $T_{\textrm{N-Gd}} =$ 2.10(2) K. Taking into account the temperature-(in)dependent components of Cr$^{3+}$ moments, we obtained an ideal model for describing the paramagnetic behavior of Gd$^{3+}$ ions within 30--140 K. We observed a magnetic reversal (positive $\rightarrow$ negative $\rightarrow$ positive) at 50 Oe with a minimum centering around 162 K. In the studied temperature range of 1.8-300 K, there exists a strong competition between magnetic susceptibilities of Gd$^{3+}$ and Cr$^{3+}$ ions, leading to puzzling magnetic phenomena. We have built the magnetic-field-dependent phase diagrams of $T_{\textrm{N-Gd}}$, $T_{\textrm{SR}}$, and $T_{\textrm{N-Cr}}$, shedding light on the nature of the intriguing magnetism. Moreover, we calculated the magnetic entropy change and obtained a maximum value at 6 K and ${\Delta}{\mu}_0H$ = 14 T, i.e., -${\Delta}S_{\textrm{M}} \approx$ 57.5 J/kg K. Among all RCrO$_3$ (R = $4f^n$ rare earths, $n =$ 7-14) compounds, the single-crystal GdCrO$_3$ compound exhibits the highest magnetic entropy change, as well as an enhanced adiabatic temperature, creating a prominent magnetocaloric effect for potential application in magnetic refrigeration., Comment: 11 pages, 5 figures

We report on single-crystal growths of the SrTb$_2$O$_4$ compound by a super-necking technique with a laser-floating-zone furnace and study the stoichiometry, growth mode, and structural and magnetic properties by scanning electronic microscopy, neutron Laue, X-ray powder diffraction, and the physical property measurement system. We optimized the growth parameters, mainly the growth speed, atmosphere, and the addition of a Tb$_4$O$_7$ raw material. Neutron Laue diffraction displays the characteristic feature of a single crystal. Our study reveals an atomic ratio of Sr:Tb $ = 0.97(2){:}2.00(1)$ and a possible layer by layer crystal growth mode. Our X-ray powder diffraction study determines the crystal structure, lattice constants and atomic positions. The paramagnetic (PM) Curie--Weiss (CW) temperature $\theta_{\texttt{CW}} =$ 5.00(4) K, and the effective PM moment $M^{\texttt{eff}}_{\texttt{mea}} =$ 10.97(1) $\mu_\texttt{B}$ per Tb$^{3+}$ ion. The data of magnetization versus temperature can be divided into three regimes, showing a coexistence of antiferromagnetic and ferromagnetic interactions. This probably leads to the magnetic frustration in the SrTb$_2$O$_4$ compound. The magnetization at 2 K and 14 T originates from both the Tb1 and Tb2 sites and is strongly frustrated with an expected saturation field at $\sim$41.5 T, displaying an intricate phase diagram with three ranges., Comment: 19 pages, 13 figures

In layered LiNixMnyCozO2 cathode material for lithium-ion batteries, the spins of transition metal (TM) ions construct a two-dimensional triangular networks, which can be considered as a simple case of geometrical frustration. By performing neutron powder diffraction experiments and magnetization measurements, we find that long-range magnetic order cannot be established in LiNixMnyCozO2 even at low temperature of 3 K. Remarkably, the frustration parameters of these compounds are estimated to be larger than 30, indicating the existence of strongly frustrated magnetic interactions between spins of TM ions. As frustration will inevitably give rise to lattice instability, the formation of Li/Ni exchange in LiNixMnyCozO2 will help to partially relieve the degeneracy of the frustrated magnetic lattice by forming a stable antiferromagnetic state in hexagonal sublattice with nonmagnetic ions located in centers of the hexagons. Moreover, Li/Ni exchange will introduce 180{\deg} superexchange interaction, which further relieves the magnetic frustration through bringing in new exchange paths. Thus, the variation of Li/Ni exchange ratio vs. TM mole fraction in LiNixMnyCozO2 with different compositions can be well understood and predicted in terms of magnetic frustration and superexchange interactions. This provides a unique viewpoint to study the Li/Ni ions exchange in layered Li(NixMnyCoz)O2 cathode materials., Comment: 22 pages, 4 figures

We report an extensive study on the zero field ground state of a powder sample of the pyrochlore $\mathrm{Yb_2Ti_2O_7}$. A sharp heat capacity anomaly that labels a low temperature phase transition in this material is observed at 280 mK. Neutron diffraction shows that a \emph{quasi-collinear} ferromagnetic order develops below $T_\mathrm{c}$ with a magnetic moment of $0.87(2)\mu_\mathrm{B}$. High resolution inelastic neutron scattering measurements show, below the phase transition temperature, sharp gapped low-lying magnetic excitations coexisting with a remnant quasielastic contribution likely associated with persistent spin fluctuations. Moreover, a broad inelastic continuum of excitations at $\sim0.6$ meV is observed from the lowest measured temperature up to at least 2.5 K. At 10 K, the continuum has vanished and a broad quasielastic conventional paramagnetic scattering takes place at the observed energy range. Finally, we show that the exchange parameters obtained within the framework of linear spin-wave theory do not accurately describe the observed zero field inelastic neutron scattering data., Comment: 11 pages, 9 figures, Phys. Rev. B. (accepted)

Ba2Ti2Fe2As4O is a self-doped superconductor exhibiting a Tc ~ 21.5 K and containing, distinctively with respect to other Fe-based superconductors, not only [Fe2As2] layers but also conducting [Ti2O] sheets. This compound exhibits a transition at T* ~ 125 K which has tentatively been assigned in the literature to a possible density-wave order. However, the nature of this density wave (whether it is a charge- or spin-induced) is still under debate. Magnetism in Ba2Ti2Fe2As4O has never been experimentally confirmed, which raises the question whether this superconductor might be non-magnetic or exhibiting a very weak magnetism. Here, we report evidence from inelastic neutron scattering (INS) measurements and ab initio calculations of phonon spectra pointing towards absence of magnetism in Ba2Ti2Fe2As4O. The INS measurements did not reveal any noticeable change of the phonon spectra across Tc, neither could magnetic effects be observed within the accessible (Q, E) space, setting Ba2Ti2Fe2As4O as an unconventional superconductor. The effect of magnetism on describing phonon spectra was further investigated by performing ab initio calculations. In this context, non-magnetic calculations reproduced well the measured phonon spectra. Therefore, our results indicate a non-magnetic and unconventional character of the superconductor Ba2Ti2Fe2As4O.

The magnetic-field-induced assembly of magnetic nanoparticles (NPs) provides a unique and flexible strategy in the design and the fabrication of functional nanostructures and devices. We have investigated the field-driven self-assembly of core-shell magnetite NPs dispersed in toluene by means of in situ small angle neutron scattering (SANS). The form factor of the core-shell NPs was characterized and analyzed using SANS with polarized neutrons. Large-scale aggregation of magnetite NPs has formed above 0.02 T as indicated by very-small angle neutron scattering measurements. Three-dimensional long-range ordered superlattice of magnetite NPs was revealed under the application of moderate magnetic field. The crystal structure of the superlattice has been identified as a face-centered cubic one., Comment: 15 pages, 7 figures

We have studied the crystal and magnetic structures of Fe-doped hexagonal manganites LuMn1-xFexO3 (x = 0, 0.1, 0.2, and 0.3) by using bulk magnetization and neutron powder diffraction methods. The samples crystalize consistently in a hexagonal structure and maintain the space group P63cm from 2 to 300 K. The N\'eel temperature TN increases continuously with increasing Fe-doping. In contrast to a single {\Gamma}4 representation in LuMnO3, the magnetic ground state of the Fe-doped samples can only be described with a spin configuration described by a mixture of {\Gamma}3 (P63'cm') and {\Gamma}4 (P63'c'm) representations, whose contributions have been quantitatively estimated. The drastic effect of Fe-doping is highlighted by composition-dependent spin reorientations. A phase diagram of the entire composition series is proposed based on the present results and those reported in literature. Our result demonstrates the importance of tailoring compositions in increasing magnetic transition temperatures of multiferroic systems., Comment: 18 pages, 9 figures

Strong spin-lattice coupling and prominent frustration effects observed in the 50$\%$ Fe-doped frustrated hexagonal ($h$)LuMnO$_3$ are reported. A N\'{e}el transition at $T_{\mathrm N} \approx$ 112~K and a possible spin re-orientation transition at $T_{\mathrm {SR}} \approx$ 55~K are observed in the magnetization data. From neutron powder diffraction data, the nuclear structure at and below 300~K was refined in polar $P6_3cm$ space group. While the magnetic structure of LuMnO$_3$ belongs to the $\Gamma_4$ ($P6'_3c'm$) representation, that of LuFe$_{0.5}$Mn$_{0.5}$O$_3$ belongs to $\Gamma_1$ ($P6_3cm$) which is supported by the strong intensity for the $\mathbf{(100)}$ reflection and also judging by the presence of spin-lattice coupling. The refined atomic positions for Lu and Mn/Fe indicate significant atomic displacements at $T_{\mathrm N}$ and $T_{\mathrm {SR}}$ which confirms strong spin-lattice coupling. Our results complement the discovery of room temperature multiferroicity in thin films of $h$LuFeO$_3$ and would give impetus to study LuFe$_{1-x}$Mn$_x$O$_3$ systems as potential multiferroics where electric polarization is linked to giant atomic displacements.

Magnetoresistance (MR) has attracted tremendous attention for possible technological applications. Understanding the role of magnetism in manipulating MR may in turn steer the searching for new applicable MR materials. Here we show that antiferromagnetic (AFM) GdSi metal displays an anisotropic positive MR value (PMRV), up to $\sim$ 415%, accompanied by a large negative thermal volume expansion (NTVE). Around $T_\text{N}$ the PMRV translates to negative, down to $\sim$ -10.5%. Their theory-breaking magnetic-field dependencies [PMRV: dominantly linear; negative MR value (NMRV): quadratic] and the unusual NTVE indicate that PMRV is induced by the formation of magnetic polarons in 5$d$ bands, whereas NMRV is possibly due to abated electron-spin scattering resulting from magnetic-field-aligned local 4$f$ spins. Our results may open up a new avenue of searching for giant MR materials by suppressing the AFM transition temperature, opposite the case in manganites, and provide a promising approach to novel magnetic and electric devices.