We investigate the ultra-sharp jump in the isothermal magnetization and the resistivity in the polycrystalline $Sm_{0.5}(Ca_{0.5-y}Sr_{y})MnO_3$ $(y = 0, 0.1, 0.2, 0.25, 0.3, 0.5)$ compounds. The critical field $(H_{cr})$, required for the ultra-sharp jump, decreases with increase of `Sr' concentration, i.e. with increase of average A-site ionic radius $\langle r_A\rangle$. The magnetotransport data indicate that the phase separation increases with the increase of $\langle r_A\rangle$, i.e. with $y$. The dependency of $H_{cr}$ with magnetic field sweep rate reveals that the ultra-sharp jump from antiferromagnetic (AFM) state to the ferromagnetic (FM) state is of martensitic in nature. Our two-band double exchange model Hamiltonian calculations show that the `Sr' doping induces the ferromagnetic clusters in the antiferromagnetic insulating phase and in turn reduces the critical field. In the end we present a phenomenological picture obtained from our combined experimental and theoretical study.
Large magnetoresistive materials are of immense interest for a number of spintronic applications by developing high density magnetic memory devices, magnetic sensors and magnetic switches. Colossal magnetoresistance, for which resistivity changes several order of magnitude (${\sim10^4 \%}$) in an external magnetic field, occurs mainly in phase separated oxide materials, namely manganites, due to the phase competition between the ferromagnetic metallic and the antiferromagnetic insulating regions. Can one further enhance the magnetoresistance by tuning the volume fraction of the two phases? In …
We investigate the behavior of ultrasharp metamagnetic transitions in La(5/8-y)Nd(y)Ca(3/8)MnO(3) manganites. These compounds change from a low temperature ferromagnetic metallic state at low Nd doping to a charge-ordered antiferromagnetic insulator for high Nd content. At an intermediate doping a phase-separated state is established. At low temperatures (2 K), we observe an avalanche-like field-induced metamagnetic transition, when the entire compound changes abruptly from one phase to the other. We investigate the signatures of this ultrasharp transition using magnetization and specific heat…
Ab initio calculations of the electric polarization of correlation-driven insulating materials, namely Mott insulators, have not been possible so far. Using a combination of density functional theory and dynamical-mean-field theory we study the electric polarization of the Mott insulator Sr$_{0.5}$Ba$_{0.5}$MnO$_{3}$. We predict a ferroelectric polarization of $\simeq 16.5 μC/cm^2$ in the high temperature paramagnetic phase and recover the measured value of $\simeq 13.3 μC/cm^2$ in the low temperature antiferromagnetic phase. Our calculations reveal that the driving force for the ferroelectric…
Magnetic, linear thermal expansion (LTE), anisotropic ($λ_t$) and volume ($ω$) magnetostriction properties of Pr$_{0.5}$Sr$_{0.5}$MnO$_3$ were investigated. The LTE decreases smoothly from 300 K without a clear anomaly either around the Curie (T$_C$ = 270 K) or the Neel temperature (T$_N$ = 100 K) and it exhibits hysteresis over a wide temperature range (60 K-270 K) upon warming. Isothermal magnetization study suggests that 13 % of the ferromagnetic phase coexists with 87 % of the antiferromagnetic phase at 25 K. The parallel and perpendicular magnetostrictions undergo rapid changes during the…
Layered LiMnO$_2$ and Li$_2$MnO$_3$ are of great interest for lithium-ion battery cathodes because of their high theoretical capacities. The practical application of these materials is, however, limited due to poor electrochemical performance. We herein report a comprehensive first-principles study of defect physics in LiMnO$_2$ and Li$_2$MnO$_3$ using hybrid-density functional calculations. We find that manganese antisites have low formation energies in LiMnO$_2$ and may act as nucleation sites for the formation of impurity phases. The antisites can also occur with high concentrations in Li$_…
We have demonstrated the effect of pressure on the steplike metamagnetic transition and its associated magnetostriction in (Eu$_{1-x}$Gd$_{x}$)$_{0.6}$Sr$_{0.4}$MnO$_{3}$ ($x=0$ and 0.1). The critical field initiating the field induced ferromagnetic transition in both samples is lowered by the applied pressure. The further application of external pressure up to 1.2 GPa on the $x=0$ parent sample causes a spontaneous ferromagnetic transition with a second-oder like character, leading to collapses of the steplike transition and its concomitant lattice striction. These findings indicate a crucial…
We have investigated the shifts of the core-level photoemission spectra of La$_{0.6}$Sr$_{0.4}$MnO$_3$ thin films grown on three kinds of substrates, SrTiO$_3$, (LaAlO$_3$)$_{0.3}$-(SrAl$_{0.5}$Ta$_{0.5}$O$_3$)$_{0.7}$, and LaAlO$_3$. The experimental shifts of the La 4d and Sr 3d core levels are almost the same as the calculation, which we attribute to the absence of covalency effects on the Madelung potentials at these atomic sites due to the nearly ionic character of these atoms. On the other hand, the experimental shifts of the O $1s$ and Mn $2p$ core levels are negligibly small, in disagr…
Relative $K$ x-ray intensities of $Mn$ in $Mn$, $MnO_{2}$, $LaMnO_{3}$ and $La_{0.7}B_{0.3}MnO_{3}$ ($B$ = $Ca$, $Sr$, and $Ce$) systems have been measured following excitation by 59.54 keV $γ$-rays from a 200 mCi $^{241}$Am point-source. The measured results for the compounds deviate significantly from the results of pure $Mn$. Comparison of the experimental data with the multiconfiguration Dirac-Fock (MCDF) effective atomic model calculations indicates reasonable agreement with the predictions of ionic model for the doped {manganites except} that the electron doped $La_{0.7}Ce_{0.3}MnO_{3}$ …
The dynamics of electrons, spins and phonons induced by optical femtosecond pulses has been simulated for the polaronic crystal $\rm{Pr_{1/2}Ca_{1/2}MnO_3}$. The model used for the simulation has been derived from first-principles calculations. The simulations reproduce the experimentally observed melting of charge/orbital order with increasing fluence. The loss of charge order in the high-fluence regime induces a transition to a ferromagnetic metal. At low fluence, the dynamics is deterministic and coherent phonons are created by the repopulation of electronic orbitals, which are strongly cou…
Two-dimensional (2D) materials are suitable hosts for the intercalation of extrinsic guest ions such as Li+, Na+ and K+ as the interlayer coupling is weak. This allows ion intercalation engineering of 2D materials, which may be a key to advancing technological applications in energy storage, neuromorphic electronics, and bioelectronics. However, ions that are extrinsic to the host materials possess challenges in fabrication of devices as there are extra steps of ion intercalation. This results in degradation of the long-term stability of the intercalated atomically thin structures. Here, we in…
The discovery of novel structural and physical properties in the $A$-site ordered manganite $R$BaMn$_{2}$O$_{6}$ ($R$ = Y and rare earth elements) has demanded new comprehension about perovskite manganese oxides. In the present study, the $A$-site disordered form, $R_{0.5}$Ba$_{0.5}$MnO$_{3}$, has been investigated and compared with both $R$BaMn$_{2}$O$_{6}$ and $R_{0.5}A_{0.5}$MnO$_{3}$ ($A$: Sr, Ca) in the structures and electromagnetic properties. $R_{0.5}$Ba$_{0.5}$MnO$_{3}$ has a primitive cubic perovskite cell in the structure and magnetic glassy states are dominant as its ground state, …
We have calculated the maximally-localized Wannier functions of MnO in its antiferromagnetic (AFM) rhombohedral unit cell, which contains two formula units. Electron Bloch functions are obtained with the linearized augmented plane-wave method within both the LSD and the LSD+U schemes. The thirteen uppermost occupied spin-up bands correspond in a pure ionic scheme to the five Mn 3d orbitals at the Mn_1 (spin-up) site, and the four O 2s/2p orbitals at each of the O_1 and O_2 sites. Maximal localization identifies uniquely four Wannier functions for each O, which are trigonally-distorted sp^3-lik…
We report a detailed study of the electric transport and magnetic properties of the LaNdCaMnO manganite system. Substitution of LaIII by smaller NdIII ions, reduces the mean ionic radius of the A site ion. We have studied samples in the entire range between rich La and rich Nd compounds. Results of DC magnetization and resistivity show that doping destabilize the FM character of the pure La compound and triggers the formation of a phase separated state at intermediate doping. We have also found evidence of a dynamical behaviour within the phase separated state. A phase diagram is constructed, …
Magnetic ground state, critical analysis of magnetization, and large magnetocaloric effect in the ferromagnetically coupled kagome lattice YCa$_3$(MnO)$_3$(BO$_3$)$_4$
Versatile features of impurity doping effects on perovskite manganites, $R_{0.6}$Sr$_{0.4}$MnO$_{3}$, have been investigated with varying the doing species as well as the $R$-dependent one-electron bandwidth. In ferromagnetic-metallic manganites ($R$=La, Nd, and Sm), a few percent of Fe substitution dramatically decreases the ferromagnetic transition temperature, leading to a spin glass insulating state with short-range charge-orbital correlation. For each $R$ species, the phase diagram as a function of Fe concentration is closely similar to that for $R_{0.6}$Sr$_{0.4}$MnO$_{3}$ obtained by de…
We studied the correlation between magnetic, electrical, structural, and magnetostriction properties of the electron doped manganites Ca$_x$Sm$_{1-x}$MnO$_3$ (x = 0.85, 0.8). The paramagnetic to antiferromagnetic transition in both the compounds while cooling is accompanied by an abrupt increase of the spontaneous volume thermal expansion ($Δ$V/V = 0.07 % for x = 0.85 and 0.25 % for x = 0.2). The x = 0.15 exhibits multiple phase separation at 5 K: G-type, and C-type antiferromagnetic phases in orthorhombic (\QTR{it}{Pnma}) and monoclinic (\QTR{it}{P2}$_1$\QTR{it}{/m}) structures respectively. …
CHGNet: Pretrained universal neural network potential for charge-informed atomistic modeling
University of California, Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；University of Cambridge（剑桥大学）；University of Minnesota（明尼苏达大学）
Co10Ge3O16 crystallizes in an intergrowth structure featuring alternating layers of spinel and rock salt. Variable-temperature powder synchrotron X-ray and neutron diffraction, magnetometry, and heat capacity experiments reveal a magnetostructural transition at T_N = 203 K. This rhombohedral-to-monoclinic transition involves a slight elongation of the CoO6 octahedra along the apical axis. Below T_N, the application of a large magnetic field causes a reorientation of the Co^2+ Ising spins. This metamagnetic transition is first-order as evidenced by a latent heat observed in temperature-dependen…
