Tetragonal distorted spinel of CuMn2-xTixO4 (x = 0, 0.25 and 0.50) was prepared by solid state reaction method followed by neutron diffraction, FTIR spectroscopy, dielectric spectroscopy and magnetization measurements. The neutron diffraction and FTIR spectroscopy provide the information regarding phase formation. But, the magnetic susceptibility clearly shows the ferri-magnetic order below 76K associated with meta-magnetic state which turns to spin-glass behaviour upon Ti-substitution for Mn in CuMn2O4. In addition, the room temperature M(H) of all the spinels are described by the Arrott's plot for weak ferromagnetism. Further, the room temperature dielectric measurement provides the electronic property of CuMn2O4 dominated by grain boundary effect that is significantly increased upon Ti-substitution for Mn in CuMn2O4.
The glass-formation range of bulk metallic glasses (BMGs) based on lanthanum and cerium was pinpointed in La-Al-Co, Ce-Al-Co and pseudo-ternary (La-Ce)-Al-Co system respectively by copper mold casting. Through the stepwise substitution of La for solvent Ce in (LaxCe1-x)65Al10Co25 alloys (0<x<1), the fully glassy rods of the (La0.7Ce0.3)65Al10Co25 alloy can be successfully produced up to 25 mm in diameter by tilt-pour casting. Comparing with the glass-forming ability (GFA) of single-lanthanide based alloys, La65Al10Co25 and Ce65Al10Co25, the coexistence of La and Ce with similar atomic size and…
The exchange bias (EB) in LaMn_{0.7}Fe_{0.3}O_3 is observed by the negative shift and training effect of the hysteresis loops, while the sample was cooled in external magnetic field. The analysis of cooling field dependence of EB gives the size of the ferromagnetic (FM) cluster ~ 25 Angstrom, where the magnetic anisotropy of FM cluster is found two order of magnitude higher than the FM bulk manganites. We propose that the nanoscale FM clusters are embedded in the glassy magnetic host with EB at the FM/glassy magnetic interface.
An effort is made to study the contrast in magnetic behavior resulting from minimal disorder introduced by substitution of 2.5% Ga or Al in Mn-site of La${_{0.9}}$Sr$_{0.1}$MnO${_3}$. It is considered that Ga or Al selectively creates disorder within the orbital domains or on its walls, causing enhancement of Griffiths phase (GP) singularity for the former and disappearance of it in the later case. It is shown that Ga replaces Mn$^{3+}$ which is considered to be concentrated within the domains, whereas Al replaces Mn$^{4+}$ which is segregated on the hole-rich walls, without causing any signif…
Nanocrystalline metals contain a large fraction of high-energy grain boundaries, which may be considered as glassy phases. Consequently, with decreasing grain size, a crossover in the deformation behaviour of nanocrystals to that of metallic glasses has been proposed. Here, we study this crossover using molecular dynamics simulations on bulk glasses, glass-crystal nanocomposites, and nanocrystals of Cu64Zr36 with varying crystalline volume fractions induced by long-time thermal annealing. We find that the grain boundary phase behaves like a metallic glass under constraint from the abutting cry…
Electronic orderings of charges, orbitals and spins are observed in many strongly correlated electron materials, and revealing their dynamics is a critical step toward understanding the underlying physics of important emergent phenomena. Here we use time-resolved resonant soft x-ray scattering spectroscopy to probe the dynamics of antiferromagnetic spin ordering in the manganite Pr$_{0.7}$Ca$_{0.3}$MnO$_3$ following ultrafast photo-exitation. Our studies reveal a glass-like recovery of the spin ordering and a crossover in the dimensionality of the restoring interaction from quasi-1D at low pum…
The magnetic and magnetotransport properties of single crystalline La1-x-yPryCaxMnO3 (x=0.42, y=0.40) thin films (~140 nm) deposited on (110) oriented LaAlO3 and SrTiO3 substrates exhibit a crossover from the high temperature antiferromagnetic-charge ordered insulator (AFM-COI) phase (T>TN) to strain glass (T<Tg). At intermediate temperatures (Tg<T<TN) dynamical liquid having prominent thermal-magneto-resistive hysteresis dominates in the cooling cycle, while in the warming cycle it is preceded by ferromagnetic metal (FMM) phase. Magnetic field required to drive AFM-COI to FMM phase transition…
Structure and magnetic properties of the compounds $Zn_{1-x}Cu_xCr_2O_4$ (ZCCO) are investigated systematically. A structural phase transition from space-group symmetry $Fd3m$ to $I4_1/amd$ is observed in ZCCO. The critical value of the doping, $x$, appears at $0.58\sim 0.62$ through the appearance of a splitting of diffraction peaks at room temperature. Measurements of dc magnetization, ac susceptibility, memory effect and exchange bias-like (EB-like) effect have been performed to reveal the glassy magnetic behaviors of ZCCO. The system with $x\leqslant 0.50$ is suggested as a spin glass-like…
The fragile-to-strong crossover seems to be a general feature of metallic glass-forming liquids. Here, we study the behavior of shear viscosity, diffusion coefficient and vibrational density of states for Cu$_\text{x}$Zr$_\text{x}$Al$_{\text{100-2x}}$ alloy through molecular dynamics simulations. The results reveal that the fragile-to-strong temperature (T$_\text{fs}$) and the glass transition temperature (T$_\text{g}$) increase as the aluminum content becomes larger. The inverse of the diffusion coefficient as a function of temperature exhibits a dynamical crossover in the vicinity of T$_\tex…
We report the structural, magnetic, transport and electronic properties of Nb substituted LaCo$_{1-x}$Nb$_x$O$_3$ ($x =$ 0--0.2). The Rietveld analysis of x-ray diffraction data demonstrate structural phase transitions from rhombohedral to orthorhombic and further to monoclinic with increasing the Nb concentration up to $x \ge$ 0.2. Interestingly, we observed dramatic changes in the magnetization (M) with increasing the Nb concentration, as the M sharply increases below 10~K even at 2.5\% substitution. Furthermore, ac susceptibility data show the spin-glass behavior in $x=$ 0.1 sample. We find…
Substitution of La by Sr in the 25% Ni doped charge transfer insulator LaFeO3 creates structural changes that inflect the electrical conductivity caused by small polaron hopping via exchange interactions and charge transfer. The substitution forms electron holes and a structural crossover from orthorhombic to rhombohedral symmetry, and then to cubic symmetry. The structural crossover is accompanied by a crossover from Fe3+-O2--Fe3+ superexchange interaction to Fe3+-O2--Fe4+ double exchange interaction, as evidenced by a considerable increase of conductivity. These interactions and charge trans…
The Arrhenius crossover temperature, $T_{A}$, corresponds to a thermodynamic state wherein the atomistic dynamics of a liquid becomes heterogeneous and cooperative; and the activation barrier of diffusion dynamics becomes temperature-dependent at temperatures below $T_{A}$. The theoretical estimation of this temperature is difficult for some types of materials, especially silicates and borates. In these materials, self-diffusion as a function of the temperature $T$ is reproduced by the Arrhenius law, where the activation barrier practically independent on the temperature $T$. The purpose of th…
In this report, the magnetic behaviour of $NiCr_{2}O_{4}$ bulk and nanoparticle samples under different applied magnetic field has been investigated extensively. Nanoparticles of $NiCr_{2}O_{4}$ were obtained by mechanical milling of polycrystalline powder prepared by polyol method. FC-ZFC measurement of bulk at different applied magnetic field has revealed the existence of a ferrimagnetic transition around 66K followed by an antiferromagnetic transition close to 30K. However, its nano counterpart has shown remarkable change in magnetic properties - a suppression of ferrimagnetic transition ac…
The comparative study of the substitution of zinc and lithium for iron in the "114" ferrites, YBaFe4O7 and CaBaFe4O7, shows that these diamagnetic cations play a major role in tuning the competition between ferrimagnetism and magnetic frustration in these oxides. The substitution of Li or Zn for Fe in the cubic phase YBaFe4O7 leads to a structural transition to a hexagonal phase YBaFe4-xMxO7, for M = Li (0.30 < x < 0.75) and for M = Zn (0.40 < x < 1.50). It is seen that for low doping values i.e. x = 0.30 (for Li) and x = 0.40 (for Zn), these diamagnetic cations induce a strong ferrimagnetic c…
In stark contrast with the conventional understanding of the glass transition, where the transition from glass to liquid appears as a dynamic process where atoms/molecules cooperatively relax into the equilibrium phase, we experimentally show that the nature of the glass transition depends at a given temperature on the ratio between the relaxation time of the glass, τ_glass, taken as its transformation time, and the alpha relaxation time, τ_α. Although the relaxation of liquid-cooled glasses is not totally synchronous, due to the existence of a distribution of relaxation times, there has been …
Magnetic properties of heterometallic warwickites $MgFeBO_4$, $Mg_{0.5}Co_{0.5}FeBO_4$, and $CoFeBO_4$ are presented, highlighting the effect of Co substitution on the magnetic properties of these compounds. The analysis of magnetization and heat capacity data has shown that these compounds exhibit a spin-glass transition below $T_{SG}$=10, 20 and 22 K, respectively. Using zero field ac susceptibility as entanglement witness we find that the low dimensional magnetic behavior above $T_{SG}$ show quantum entanglement behavior $χ(T)\varpropto T^{-α(T)}$ up to $T_E$ = 130K. The $α$ parameters have…
The study of the ferrites YBaFe4-xGaxO7 shows that the substitution of Ga for Fe in YBaFe4O7 stabilizes the hexagonal symmetry for 0.40 < x < 0.70, at the expense of the cubic one. Using combined measurements of a. c. and d. c. magnetization, we establish that Ga substitution for Fe in YBaFe4O7 leads to an evolution from a geometrically frustrated spin glass (for x = 0) to a cationic disorder induced spin glass (x = 0.70). We also find an intermediate narrow range of doping where the samples are clearly phase separated having small ferrimagnetic clusters embedded in a spin glass matrix. The or…
Silica is known as the archetypal strong liquid, exhibiting an Arrhenius viscosity curve with a high glass transition temperature and constant activation energy. However, given the ideally isostatic nature of the silica network, the presence of even a small concentration of defects can lead to a significant decrease in both the glass transition temperature and activation energy for viscous flow. To understand the impact of trace level dopants on the viscosity of silica, we measure the viscosity-temperature curves for seven silica glass samples having different impurities, including four natura…
Physical properties of partially Ca substituted hole-doped Dy2Ti2O7 have been investigated by ac magnetic susceptibility χ_ac(T), dc magnetic susceptibility χ(T), isothermal magnetization M(H) and heat capacity C_p(T) measurements on Dy1.8Ca0.2Ti2O7. The spin-ice system Dy2Ti2O7 exhibits a spin-glass type freezing behavior near 16 K. Our frequency dependent χ_ac(T) data of Dy1.8Ca0.2Ti2O7 show that the spin-freezing behavior is significantly influenced by Ca substitution. The effect of partial nonmagnetic Ca2+ substitution for magnetic Dy3+ is similar to the previous study on nonmagnetic isova…
Antiferromagnetic Bi_{2}Fe_{4}O_{9} (BFO), lightly substituted by cobalt is studied for magnetodielectricity. The substitution causes a substantial decrease in the Neel temperature (T_N) from 250 K (in parent sample, BFO) to 152 K (in 2% Co substituted sample). At the same time, the substituted samples display a pronounced irreversibility in the ZFC-FC magnetization data for T $<$ 370 K and opening of hysteresis in the M-H plot, thus signifying the onset of weak ferromagnetism (FM) and magnetic glassiness. The induced magnetic glassiness is found to slow down the dynamics such that the magneti…
The substitution of zinc for iron in YBaFe4O7 has allowed the oxide series YBaFe4-xZnxO7, with 0.40 < x < 1.50, belonging to the "114" structural family to be synthesized. These oxides crystallize in the hexagonal symmetry (P63mc), as opposed to the cubic symmetry (F-43m) of YBaFe4O7. Importantly, the d.c. magnetization shows that the zinc substitution induces ferrimagnetism, in contrast to the spin glass behaviour of YBaFe4O7. Moreover, a.c. susceptibility measurements demonstrate that concomitantly these oxides exhibit a spin glass or a cluster glass behaviour, which increases at the expense…
We demonstrate that recent experimental data (E. Castel et al J.Phys. Cond. Mat. {\bf 21} (2009), 452201) on tungsten bronze compound (TBC) Ba$_2$Pr$_x$Nd$_{1-x}$FeNb$_4$O$_{15}$ can be well explained in our model predicting a crossover from ferroelectric ($x=0$) to orientational (dipole) glass ($x=1$), rather then relaxor, behavior. We show, that since a "classical" perovskite relaxor like Pb(Mn$_{1/3}$ Nb$_{2/3}$)O$_3$ is never a ferroelectric, the presence of ferroelectric hysteresis loops in TBC shows that this substance actually transits from ferroelectric to orientational glass phase wit…
Non-Monotonic Dynamical Correlations Across The Glass Crossover
Eindhoven University of Technology（埃因霍温理工大学）；Institute for Complex Molecular Systems, Eindhoven University of Technology（埃因霍温理工大学复杂分子系统研究所）；Deutsches Zentrum für Luftund Raumfahrt (DLR)（德国航空航天中心）；Heinrich-Heine-Universität Düsseldorf（杜塞尔多夫大学）；Institute of Complex Systems (ISC) - CNR, Rome unit（罗马复杂系统研究所（国家研究委员会））；Sapienza Università di Roma（罗马第一大学）；Istituto Nazionale di Fisica Nucleare, Sezione di Roma I（意大利国家核物理研究所罗马一分部）
Results of low temperature dielectric measurements on the mixed (Ca_(1-x)Pb_(x))TiO_(3) system are presented to show that a dielectric anomaly appears for x \geq 0.10. The observed dielectric peak is shown to be due to a thermodynamic phase transition and not due to a relaxor or dipole glass type transition. Curie-Weiss fit to the dielectric constant gives negative Curie temperature which points towards an antiferroelectric transition. Arguments are advanced to propose that CaTiO3 may be an incipient antiferroelectric in which Pb^(2+) substitution stabilises the antiferroelectric phase.
The existence of a 'crossover region' in glass-forming liquids has long been considered as a general phenomenon that is as important as the glass transition. One potential origin for the crossover behavior is a liquid-to-liquid phase transition (LLPT). Although a LLPT is thought to exist in all forms of liquids, structural evidence for this, particularly in supercooled liquids, is scarce, elusive, and in many cases controversial. A key challenge to the search for a LLPT in a supercooled liquid is the interference of crystallization during cooling. Crystallization induces major structural chang…
We report new time-resolved synchrotron x-ray diffraction (SXRD) measurements to track structural transformations in calcium-aluminate (CaO)x(Al2O3)1-x liquids during glass formation, and review recent progress in neutron diffraction with isotope substitution (NDIS) experiments, combined with aspherical ion model molecular dynamics (AIM-MD) simulations, to identify the atomic-scale configurational constraints on glass-forming ability.
MgGeO$_3$-perovskite is known to be a low-pressure analog of MgSiO$_3$-perovskite in many respects, but especially in regard to the post-perovskite transition. As such, investigation of spin state changes in Fe-bearing MgGeO$_3$ might help to clarify some aspects of this type of state change in Fe-bearing MgSiO$_3$. Using DFT+U calculations, we have investigated pressure induced spin state changes in Fe$^{2+}$ and Fe$^{3+}$ in MgGeO$_3$ perovskite and post-perovskite. Owing to the relatively larger atomic size of germanium compared to silicon, germanate phases have larger unit cell volume and …
The magnetic susceptibility of the 1/1 approximants to icosahedral quasicrystals in a series of Cd85-xMgxTb15 (x = 5, 10, 15, 20) alloys was investigated in detail. The occurrence of antiferromagnetic to spin-glass-like transition was noticed by increasing Mg. Transmission electron microscopy analysis evidenced a correlation between the magnetic transition and suppression of the monoclinic superlattice ordering with respect to the orientation of the Cd4 tetrahedron at T > 100 K. The possible origins of this phenomenon were discussed in detail. The occurrence of the antiferromagnetic to spin-gl…
