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Noncollinear magnetic structures and multiple magnetic phase transitions in a sawtooth lattice antiferromagnet consisting of Cr$^{3+}$ are experimentally identified in this work, thereby proposing the scenario of magnetism-driven ferroelectricity in a sawtooth lattice. The title compound, BeCr$_2$O$_4$, displays three magnetic phase transitions at low temperatures, at $T_{N1}\approx$ 7.5 K, at $T_{N2}\approx$ 25 K and at $T_{N3}\approx$ 26 K, revealed through magnetic susceptibility, specific heat and neutron diffraction in this work. These magnetic phase transitions are found to be influenced by externally applied magnetic fields. Isothermal magnetization curves at low temperatures below the magnetic transitions indicate the antiferromagnetic nature of \bco\ with two spin-flop-like transitions occurring at $H_{c1}\approx$ 29 kOe and $H_{c2} \approx$ 47 kOe. Our high-resolution X-ray and neutron diffraction studies, performed on single crystal and powder samples unambiguously determined the crystal structure as orthorhombic $Pbnm$. By performing the magnetic superspace group analysis of the neutron diffraction data at low temperatures, the magnetic structure in the temperature range $T_{N3,N2} < T < T_{N1}$ is determined to be the polar magnetic space group, $P21nm.1^{\prime}(00g)0s0s$ with a cycloidal magnetic propagation vector $\textbf{k}_1$ = (0, 0, 0.090(1)). The magnetic structure in the newly identified phase below $T_{N1}$, is determined as $P21/b.1^{\prime}[b](00g)00s$ with the magnetic propagation vector $\textbf{k}_2$ = (0, 0, 0.908(1)). The cycloidal spin structure determined in our work is usually associated with electric polarization, thereby making \bco\ a promising multiferroic belonging to the sparsely populated family of sawtooth lattice antiferromagnets., Comment: 24 pages, 5 figures, accepted

We report the magnetic, electronic and transport properties of the quasi-skutterudite compound Pr$_3$Ir$_4$Ge$_{13}$ by means of magnetic susceptibility $\chi(T)$, electrical resistivity $\rho(T)$, specific heat $C_p(T)$, thermal conductivity $\kappa(T)$, thermoelectric power $S(T)$ and Hall coefficient $R_\mathrm{H}(T)$ measurements. Pr$_3$Ir$_4$Ge$_{13}$ does not show any phase transition down to 1.9 K. Magnetic, and specific measurements show that the system possesses a crystal electric field singlet ground state that is separated from the first excited state by about 37 K. $\rho(T)$ shows a negative temperature coefficient of resistance for the whole temperature range studied and which can be explained in terms of Mott's impurity band conduction mechanism. $R_\mathrm{H}(T)$ measurements show that Pr$_3$Ir$_4$Ge$_{13}$ is a low-carrier density semimetal and its transport properties indicate a metallic-non metallic cross over behaviour. Large Seebeck values were observed for the entire temperature range of investigation, and the analysis of temperature variation of $S$ and $S/T$ showed no sign of strong correlation between the Pr 4$f^2$ and conduction electron states near Fermi level. A large Sommerfeld coefficient, $\gamma = 150$~mJ/(mol K$^2$) indicates the formation of a moderate heavy-fermion state emerging from the dynamical crystal field fluctuations., Comment: 17 pages, 10 Figures

The perovskite TbFe$_{0.5}$Cr$_{0.5}$O$_3$ shows two anomalies in the magnetic susceptibility at $T_N$ = 257K and $T_{SR}$ = 190K which are respectively, the antiferromagnetic and spin reorientation transition that occur in the Fe/Cr sublattice. Analysis of the magnetic susceptibility reveals signatures of Griffiths-like phase in this compound. Neutron diffraction analysis confirms that, as the temperature is reduced from 350K, a spin reorientation transition from $\Gamma_2$ (F$_x$, C$_y$, G$_z$) to $\Gamma_4$ (G$_x$, A$_y$, F$_z$) occurs at $T_N$ = 257K and subsequently, a second spin reorientation takes place from $\Gamma_4$ (G$_x$, A$_y$, F$_z$) to $\Gamma_2$ (F$_x$, C$_y$, G$_z$) at $T_{SR}$ = 190K. The $\Gamma_2$ (F$_x$, C$_y$, G$_z$) structure is stable until 7.7K where an ordered moment of 7.74(1)$\mu_\mathrm B$/Fe$^{3+}$(Cr$^{3+}$) is obtained from neutron data refinement. In addition to the long-range order of the magnetic structure, indication of diffuse magnetic scattering at 7.7K is evident, thereby lending support to the Griffiths-like phase observed in susceptibility. At 7.7K, Tb develops a ferromagnetic component along the crystallographic $a$ axis. Thermal conductivity, and spin-phonon coupling of TbFe$_{0.5}$Cr$_{0.5}$O$_3$ through Raman spectroscopy are studied in the present work. An antiferromagnetic structure with ($\uparrow \downarrow \uparrow \downarrow$) arrangement of Fe/Cr spins is found in the ground state through first-principles energy calculations which supports the experimental magnetic structure at 7.7K. The spin-resolved total and partial density of states are determined showing that TbFe$_{0.5}$Cr$_{0.5}$O$_3$ is insulating with a band gap of $\sim 0.12$ (2.4) eV within GGA (GGA+$U$) functionals., Comment: 11 pages, 10 figures

PrCo$_2$Ga$_8$ is an orthorhombic quasi-skutterudite type compound which crystallizes in the CaCo$_2$Al$_8$ structure type, with space group $Pbam$ (No. 55). The Pr$^{3+}$ ion has a site symmetry of $C_s$ which predicts a crystal electric field (CEF) level splitting into 9 singlets for $J$ = 4. However, a phase transition at $T_m$ = 1.28~K is observed in electrical resistivity and specific heat results and is reported in this paper. The electrical resistivity shows an upturn below $T_m$ due to the superzone-gap formation. This transition is tuneable in fields and is suppressed to lower temperatures with applied magnetic fields. The electronic specific heat $C_{p}(T)/T$ increases below $T_m$ and reaches a value of 7.37 J/(mol K$^2$) at 0.4~K. The Sommerfeld coefficient, $\gamma$ extracted from the low temperature analysis of $C_\mathrm{4f}(T)/T$ is 637 mJ/(mol K$^2$) indicating a possible mass enhancement of the quasiparticles. The calculated entropy value of 3.05 J/(mol K) is recovered around $T_m$ exhibiting almost 53% of Rln2, where R is the universal gas constant. Magnetic susceptibility results obeys the Curie-Weiss law for data above 100 K with an estimated effective magnetic moment, $\mu_\mathrm{eff}$ = 3.37 $\mu_B$/Pr and Weiss temperature, $\theta_p$ = $-$124 K., Comment: 11 pages, 5 figures, SCES 2017 conference proceedings

We report the experimental observation of spin reorientation in the double perovskite Ho$_2$FeCoO$_6$. The magnetic phase transitions in this compound are characterized and studied through magnetization and specific heat, and the magnetic structures are elucidated by neutron powder diffraction. Two magnetic phase transitions are observed in this compound - one at $T_\mathrm{N1} \approx$ 250~K, from paramagnetic to antiferromagnetic, and the other at $T_\mathrm{N2} \approx$ 45~K, from a phase with mixed magnetic structures to a single phase through a spin reorientation process. The magnetic structure in the temperature range 200~K - 45~K is a mixed phase of the irreducible representations $\Gamma_1$ and $\Gamma_3$, both of which are antiferromagnetic. The phase with mixed magnetic structures that exists in Ho$_2$FeCoO$_6$ gives rise to a large thermal hysteresis in magnetization that extends from 200~K down to the spin reorientation temperature. At $T_\mathrm{N2}$, the magnetic structure transforms to $\Gamma_1$. Though long-range magnetic order is established in the transition metal lattice, it is seen that only short-range magnetic order prevails in Ho$^{3+}$ - lattice. Our results should motivate further detailed studies on single crystals in order to explore spin reorientation process, spin switching and the possibility of anisotropic magnetic interactions giving rise to electric polarization in Ho$_2$FeCoO$_6$.

The ternary intermetallic compound Gd$_2$Cu$_2$In crystallizes in Mo$_2$Fe$_2$B type structure with the space group $P4/mbm$ and we study critical behaviour and magnetocaloric effect near the ferromagnetic transition ($T_C$ $\approx$ 94 K) using the magnetic and heat capacity measurements. The maximum entropy change ($\Delta S_m$) and adiabatic temperature change ($\Delta T_{ad}$) for the field value of 7 T were observed to be 13.8 J/kg.K and 6.5 K respectively. We have employed modified Arrott plot (MAP), Kouvel-Fisher (KF) procedures to estimate the critical exponents near the FM-PM phase transition. Critical exponents $\beta$ = 0.312(2), $\gamma$ = 1.080(5) are self-consistently estimated from the non-linear fitting. The $\beta$ value is close to the three dimensional (3D) Ising model where as $\gamma$ and $\delta$ values are close to mean field model. The estimated critical exponents for Gd$_2$Cu$_2$In suggest that the system may belong to different universal class. All the three critical exponent obey Widom scale and collapse the scaled magnetic isotherms into two distinct branches below and above $T_C$ in accordance with single scaling equation. Specific heat measurements show a $\lambda$ type peak near 94 K confirming the bulk magnetic ordering. The data near $T_C$ was fitted using the non-linear function $C_{P} = B + C\epsilon + A^{\pm}|\epsilon|^{-\alpha}(1 + E^{\pm} |\epsilon|^{0.5})$ between -0.025$<\epsilon<$0.025 which yielded the fourth critical exponent $\alpha$ value to be 0.11 (3). The value indicates possible 3D-Ising behavior where Gd$^{3+}$ moments arranged uniaxially along long tetragonel axis 'c' as reported in literature., Comment: 7 pages, double colum, 4 figures

The intermetallic compound \PFA\ that possesses a three-dimensional network structure of Al polyhedra centered at the transition metal element Fe and the rare earth Pr is investigated through neutron powder diffraction and inelastic neutron scattering in order to elucidate the magnetic ground state of Pr and Fe and the crystal field effects of Pr. Our neutron diffraction study confirms long-range magnetic order of Pr below $T_N $ = 4.5~K in this compound. Subsequent magnetic structure estimation reveals a magnetic propagation vector $k$ = ($\frac{1}{2}$~0~$\frac{1}{2}$) with a magnetic moment value of 2.5~$\mu_\mathrm{B}$/Pr along the orthorhombic $c$-axis and evidence the lack of ordering in the Fe sublattice. The inelastic neutron scattering study reveals one crystalline electric field excitation near 19~meV at 5~K in \PFA. The energy-integrated intensity of the 19~meV excitation as a function of |$Q$| $(A^{-1})$ follows the square of the magnetic form factor of Pr$^{3+}$ thereby confirming that the inelastic excitation belongs to the Pr sublattice. The second sum rule applied to the dynamic structure factor indicates only 1.6(2)~$\mu_\mathrm{B}$ evolving at the 19~meV peak compared to the 3.58~$\mu_\mathrm{B}$ for free Pr$^{3+}$, indicating that the crystal field ground state is magnetic and the missing moment is associated with the resolution limited quasi-elastic line. The magnetic order occurring in Pr in \PFA\ is counter-intuitive to the symmetry-allowed crystal field level scheme, hence, is suggestive of exchange-mediated mechanisms of ordering stemming from the magnetic ground state of the crystal field levels., Comment: 8 pages, double-column, 6 figures (accepted to J. Phys. Condens. Matter)

The double perovskite Y_2NiMnO_6 displays ferromagnetic transition at Tc = 81 K. The ferromagnetic order at low temperature is confirmed by the saturation value of magnetization (M_s) and also, validated by the refined ordered magnetic moment values extracted from neutron powder diffraction data at 10 K. This way, the dominant Mn4+ and Ni2+ cationic ordering is confirmed. The cation-ordered P 21/n nuclear structure is revealed by neutron powder diffraction studies at 300 and 10 K. Analysis of frequency dependent dielectric constant and equivalent circuit analysis of impedance data takes into account the bulk contribution to total dielectric constant. This reveals an anomaly which coincides with the ferromagnetic transition temperature (T_c). Pyrocurrent measurements register a current flow with onset near Tc and a peak at 57 K that shifts with temperature ramp rate. The extrinsic nature of the observed pyrocurrent is established by employing a special protocol measurement. It is realized that the origin is due to re-orientation of electric dipoles created by the free charge carriers and not by spontaneous electric polarization at variance with recently reported magnetism-driven ferroelectricity in this material, Comment: Published in Physical Review B

Single crystals of Frank-Kasper compounds RTM$_2$Al$_{20}$ (R = Eu, Gd and La; TM = V and Ti) were grown by self-flux method and their physical properties were investigated through magnetization ($M$), magnetic susceptibility ($\chi$), specific heat ($C_P$) and electrical resistivity ($\rho$) measurements. Powder x-ray diffraction studies and structural analysis showed that these compounds crystallize in the cubic crystal structure with the space group $Fd\overline{3}m$. The magnetic susceptibility for the compounds EuTi$_2$Al$_{20}$ and GdTi$_2$Al$_{20}$ showed a sudden jump below the N{\'e}el temperature $T_N$ indicative of plausible double magnetic transition. Specific heat ($C_P$) and electrical resistivity ($\rho$) measurements also confirm the first-order magnetic transition (FOMT) and possible double magnetic transitions. Temperature variation of heat capacity showed a sharp phase transition and huge $C_P$ value for the (Eu/Gd)Ti$_2$Al$_{20}$ compounds Full width at half-maximum (FWHM) $<$ 0.2 K) which is reminiscent of a first-order phase transition and a unique attribute among RTM$_2$Al$_{20}$ compounds. We observed clear anomaly between heating and cooling cycle in temperature-time relaxation curve for the compounds GdTi$_2$Al$_{20}$ (2.38 $K$) and EuTi$_2$Al$_{20}$ (3.2 $K$) which is indicating a thermal arrest due to the latent heat. The temperature variation of $S_{mag}$ for GdTi$_2$Al$_{20}$ saturates to a value $0.95R\ln8$ while the other magnetic systems exhibited still lower entropy saturation values in the high temperature limit. Resistivity measurements showed that all the samples behave as normal Fermi liquid type compounds and $\rho(T)$ due to electron-phonon scattering follows Bloch-Gr$\ddot{\textrm u}$neisen-Mott relation in the paramagnetic region., Comment: 13 figures, 3 Tables

Exchange bias-like effect observed in the intermetallic compound TbFeAl, which displays a magnetic phase transition at $T^h_c \approx$ 198~K and a second one at $T^l_c \approx$ 154~K, is reported. {\em Jump}-like features are observed in the isothermal magnetization, $M (H)$, at 2~K which disappear above 8~K. The field-cooled magnetization isotherms below 10~K show loop-shifts that are reminiscent of exchange bias, also supported by {\em training effect}. Significant coercive field, $H_c \approx$ 1.5~T at 2~K is observed in TbFeAl which, after an initial increase, shows subsequent decrease with temperature. The exchange bias field, $H_{eb}$, shows a slight increase and subsequent leveling off with temperature. It is argued that the inherent crystallographic disorder among Fe and Al and the high magnetocrystalline anisotropy related to Tb$^{3+}$ lead to the exchange bias effect. TbFeAl is recently reported to show magnetocaloric effect and the present discovery of exchange bias makes this compound a multifunctional one. The result obtained on TbFeAl generalizes the observation of exchange bias in crystallographically disordered materials and gives impetus for the search for materials with {\em exchange bias induced by atomic disorder.}, Comment: 4 pages, 5 figures, double-column, Accepted to Europhys. Lett., 2016

The magnetic, thermodynamic and electrical/thermal transport properties of the caged-structure quasi-skutterudite Gd$_3$Ir$_4$Sn$_{13}$ are re-investigated. The magnetization $M(T)$, specific heat $C_p(T)$ and the resistivity $\rho(T)$ reveal a double-phase transition -- at $T_{N1}\sim$ 10~K and at $T_{N2}\sim$ 8.8~K -- which was not observed in the previous report on this compound. The antiferromagnetic transition is also visible in the thermal transport data, thereby suggesting a close connection between the electronic and lattice degrees of freedom in this Sn-based quasi-skutterudite. The temperature dependence of $\rho(T)$ is analyzed in terms of a power-law for resistivity pertinent to Fermi liquid picture. Giant, positive magnetoresistance (MR) $\approx$ 80$\%$ is observed in Gd$_3$Ir$_4$Sn$_{13}$ at 2~K with the application of 9~T. The giant MR and the double magnetic transition can be attributed to the quasi-cages and layered antiferromagnetic structure of Gd$_3$Ir$_4$Sn$_{13}$ vulnerable to structural distortions and/or dipolar or spin-reorientation effects. The giant value of MR observed in this class of 3:4:13 type alloys, especially in a Gd-compound, is the highlight of this work., Comment: 20 pages single column, 7 figures, 1 table; Accepted to J. Appl. Phys., 2016

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

The robust field-insensitive heavy fermion features in Sm$_3$Ru$_4$Ge$_{13}$ and the magnetic phase transition at $T_N \approx$ 5~K are studied using magnetization $M(T)$, specific heat $C_p(T)$, resistivity $\rho(T)$ and thermal conductivity $\kappa_T(T)$. The average crystal structure of Sm$_3$Ru$_4$Ge$_{13}$ conforms to the cubic space group $Pm\bar{3}n$ however, signatures of subtle structural distortions are obtained from the x ray data. The magnetic susceptibility, $\chi(T)$, follows a modified Curie-Weiss law indicating the presence of crystal fields of Sm$^{3+}$ and the significance of van Vleck terms. No sign of ferromagnetism is observed in $M(H)$ of Sm$_3$Ru$_4$Ge$_{13}$ which yields only 0.025~$\mu_\mathrm{B}$/f.u.-Sm at 2~K, 7~T. The Sommerfeld coefficient, $\gamma \approx$ 220~mJ/mol-Sm K$^2$, estimated from the analysis of low temperature specific heat suggests the formation of heavy quasi particles at low temperature. Though a ln$T$ dependence of $\rho(T)$ is observed till 60~K, the resistivity behavior is accounted for by assuming a two-band model for activated behavior of charge carriers. The field scans of resistivity, $\rho(H)$, below $T_N$ display significant nonlinearity while those above the $T_N$ are more metal-like. Low values of thermal conductivity, $\kappa_T(T)$, are observed in Sm$_3$Ru$_4$Ge$_{13}$ however, displaying an anomaly at $T_N$ which signifies magnetoelastic coupling. A fairly high value of Seebeck coefficient, $S \approx$ 40~$\mu$V/K is observed at 300~K. We identify Sm$_3$Ru$_4$Ge$_{13}$ as a low charge carrier density system with unusual field-insensitive heavy fermion features very similar to the filled skutterudites., Comment: 18 pages, 7 figures, Accepted to J. Alloys and Comp., 2016

The magnetic structures and the magnetic phase transitions in the Mn-doped orthoferrite TbFeO$_3$ studied using neutron powder diffraction are reported. Magnetic phase transitions are identified at $T^\mathrm{Fe/Mn}_N \approx$ 295~K where a paramagnetic-to-antiferromagnetic transition occurs in the Fe/Mn sublattice, $T^\mathrm{Fe/Mn}_{SR} \approx$ 26~K where a spin-reorientation transition occurs in the Fe/Mn sublattice and $T^\mathrm{R}_N \approx$ 2~K where Tb-ordering starts to manifest. At 295~K, the magnetic structure of the Fe/Mn sublattice in TbFe$_{0.5}$Mn$_{0.5}$O$_3$ belongs to the irreducible representation $\Gamma_4$ ($G_xA_yF_z$ or $Pb'n'm$). A mixed-domain structure of ($\Gamma_1 + \Gamma_4$) is found at 250~K which remains stable down to the spin re-orientation transition at $T^\mathrm{Fe/Mn}_{SR}\approx$ 26~K. Below 26~K and above 250~K, the majority phase ($> 80\%$) is that of $\Gamma_4$. Below 10~K the high-temperature phase $\Gamma_4$ remains stable till 2~K. At 2~K, Tb develops a magnetic moment value of 0.6(2)~$\mu_\mathrm{B}/$f.u. and orders long-range in $F_z$ compatible with the $\Gamma_4$ representation. Our study confirms the magnetic phase transitions reported already in a single crystal of TbFe$_{0.5}$Mn$_{0.5}$O$_3$ and, in addition, reveals the presence of mixed magnetic domains. The ratio of these magnetic domains as a function of temperature is estimated from Rietveld refinement of neutron diffraction data. Indications of short-range magnetic correlations are present in the low-$Q$ region of the neutron diffraction patterns at $T < T^\mathrm{Fe/Mn}_{SR}$. These results should motivate further experimental work devoted to measure electric polarization and magnetocapacitance of TbFe$_{0.5}$Mn$_{0.5}$O$_3$., Comment: 16 pages, 7 figures, Accepted to J. Appl. Phys., 2016

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.

The compound PrFe$_2$Al$_8$ possesses a three-dimensional network structure resulting from the packing of Al polyhedra centered at the transition metal element Fe and the rare earth Pr. Along the $c$-axis, Fe and Pr form {\em chains} which are separated from each other by the Al-network. In this paper, the magnetism and crystalline electric field effects in PrFe$_2$Al$_8$ are investigated through the analysis of magnetization and specific heat data. A magnetic phase transition in the Pr lattice is identified at $T^{Pr}_{N}\approx$ 4~K in dc magnetization and ac susceptibility data. At 2~K, the magnetization isotherm presents a ferromagnetic saturation, however, failing to reach full spin-only ferromagnetic moment of Pr$^{3+}$. Metamagnetic step-like low-field features are present in the magnetization curve at 2~K which is shown to shift upon field-cooling the material. Arrott plots centered around $T^{Pr}_{N}$ display "S"-like features suggestive of an inhomogeneous magnetic state. The magnetic entropy, $S_m$, estimated from specific heat outputs a value of $R$ ln(2) at $T_{N2}$ suggesting a doublet state for Pr$^{3+}$. The magnetic specific heat is modeled by using a 9-level Schottky equation pertinent to the Pr$^{3+}$ ion with $J$ = 4. Given the crystalline electric field situation of Pr$^{3+}$, the inference of a doublet state from specific heat and consequent long-range magnetic order is an unexpected result., Comment: 7 Pages and 8 Figures

Orthorhombic single crystals of TbMn0.5Fe0.5O3 are found to exhibit spin-reorientation, magnetization reversal and weak ferromagnetism. Strong anisotropy effects are evident in the temperature dependent magnetization measurements along the three crystallographic axes a, b and c. A broad magnetic transition is visible at T_N (Fe/Mn) = 286 K due to paramagnetic to AxGyCz ordering. A sharp transition is observed at T_SR (Fe/Mn) = 28 K, which is pronounced along c axis in the form of a sharp jump in magnetization where the spins reorient to GxAyFz configuration. The negative magnetization observed below TSR Fe/Mn along c axis is explained in terms of domain wall pinning. A component of weak ferromagnetism is observed in field-scans along c-axis but below 28 K. Field-induced steps-like transitions are observed in hysteresis measurement along b axis below 28 K. It is noted that no sign of Tb-order is discernible down to 2 K. TbMn0.5Fe0.5O3 could be highlighted as a potential candidate to evaluate its magneto-dielectric effects across the magnetic transitions., Comment: Accepted in J. Appl. Phys

Spin freezing in the $A$-site spinel FeAl$_2$O$_4$ which is a spin liquid candidate is studied using remnant magnetization and nonlinear magnetic susceptibility and isofield cooling and heating protocols. The remnant magnetization behavior of FeAl$_2$O$_4$ differs significantly from that of a canonical spin glass which is also supported by analysis of the nonlinear magnetic susceptibility term $\chi_3 (T)$. Through the power-law analysis of $\chi_3 (T)$, a spin-freezing temperature, $T_g$ = 11.4$\pm$0.9~K and critical exponent, $\gamma$ = 1.48$\pm$0.59 are obtained. Cole-Cole analysis of magnetic susceptibility shows the presence of broad spin relaxation times in FeAl$_2$O$_4$, however, the irreversible dc susceptibility plot discourages an interpretation based on conventional spin glass features. The magnetization measured using the cooling-and-heating-in-unequal-fields protocol brings more insight to the magnetic nature of this frustrated magnet and reveals unconventional glassy behaviour. Combining our results, we arrive at the conclusion that the present sample of FeAl$_2$O$_4$ consists of a majority spin liquid phase with "glassy" regions embedded., Comment: 5 pages, 6 figs, 2-column, Accepted to Phys. Rev. B

Exchange bias effect in the ferromagnetic double perovskite compound Y$_2$CoMnO$_6$, which is also a multiferroic, is reported. The exchange bias, observed below 8~K, is explained as arising due to the interface effect between the ferromagnetic and antiferromagnetic clusters created by {\it antisite} disorder in this material. Below 8~K, prominent ferromagnetic hysteresis with metamagnetic "steps" and significant coercive field, $H_c \approx$ 10~kOe are observed in this compound which has a $T_c \approx$ 75~K. A model based on growth of ferromagnetic domains overcoming the elastic energy of structurally pinned magnetic interfaces, which closely resembles martensitic-like transitions, is adapted to explain the observed effects. The role of {\it antisite} disorder in creating the domain structure leading to exchange bias effect is highlighted in the present work., Comment: 4 pages two-column, 4 figures, accepted to Appl. Phys. Lett

We re-investigate the magnetically frustrated, {\it diamond-lattice-antiferromagnet} spinels FeAl$_2$O$_4$ and MnAl$_2$O$_4$ using magnetization measurements and diffuse scattering of polarized neutrons. In FeAl$_2$O$_4$, macroscopic measurements evidence a "cusp" in zero field-cooled susceptibility around 13~K. Dynamic magnetic susceptibility and {\it memory effect} experiments provide results that do not conform with a canonical spin-glass scenario in this material. Through polarized neutron scattering studies, absence of long-range magnetic order down to 4~K is confirmed in FeAl$_2$O$_4$. By modeling the powder averaged differential magnetic neutron scattering cross-section, we estimate that the spin-spin correlations in this compound extend up to the third nearest-neighbour shell. The estimated value of the Land\'{e} $g$ factor points towards orbital contributions from Fe$^{2+}$. This is also supported by a Curie-Weiss analysis of the magnetic susceptibility. MnAl$_2$O$_4$, on the contrary, undergoes a magnetic phase transition into a long-range ordered state below $\approx$ 40~K, which is confirmed by macroscopic measurements and polarized neutron diffraction. However, the polarized neutron studies reveal the existence of prominent spin-fluctuations co-existing with long-range antiferromagnetic order. The magnetic diffuse intensity suggests a similar short range order as in FeAl$_2$O$_4$. Results of the present work supports the importance of spin-spin correlations in understanding magnetic response of frustrated magnets like $A$-site spinels which have predominant short-range spin correlations reminiscent of the "spin liquid" state., Comment: 10 pages, 10 figures, double-column, accepted in Phys. Rev. B, 2014

Frequency-dependent and temperature-dependent dielectric measurements are performed on double perovskite Tb$_2$NiMnO$_6$. The real ($\epsilon_1$) and imaginary ($\epsilon_2$) parts of dielectric permittivity show three plateaus suggesting dielectric relaxation originating from bulk, grain boundaries and the sample-electrode interfaces respectively. The temperature and frequency variation of $\epsilon_1$ and $\epsilon_2$ are successfully simulated by a $RC$ circuit model. The complex plane of impedance, $Z'$-$Z"$, is simulated using a series network with a resistor $R$ and a constant phase element. Through the analysis of frequency-dependent dielectric constant using modified-Debye model, different relaxation regimes are identified. Temperature dependence of dc conductivity also presents a clear change in slope at, $T^*$. Interestingly, $T^*$ compares with the temperature at which an anomaly occurs in the phonon modes and the Griffiths temperature for this compound. The components $R$ and $C$ corresponding to the bulk and the parameter $\alpha$ from modified-Debye fit tend support to this hypothesis. Though these results cannot be interpreted as magnetoelectric coupling, the relationship between lattice and magnetism is marked., Comment: Accepted in Europhysics Letters

Neutron diffraction measurement on the spin glass double perovskite Sr$_2$FeCoO$_6$ reveals site disorder as well as Co$^{3+}$ intermediate spin state. In addition, multiple valence states of Fe and Co are confirmed through M\"{o}ssbauer and X-ray photoelectron spectroscopy. The structural disorder and multiple valence lead to competing ferromagnetic and antiferromagnetic interactions and subsequently to a spin glass state, which is reflected in the form of an additional $T$-linear contribution at low temperatures in specific heat. A clear evidence of Jahn-Teller distortion at the Co$^{3+}$-O$_6$ complex is observed and incorporating the physics of Jahn-Teller effect, the presence of localized magnetic moment is shown. A large, negative and anomalous magnetoresistance of $\approx$ 63% at 14K in 12T applied field is observed for Sr$_2$FeCoO$_6$. The observed magnetoresistance could be explained by applying a semi-empirical fit consisting of a negative and a positive contribution and show that the negative magnetoresistance is due to spin scattering of carriers by localized magnetic moments in the spin glass phase.

We have investigated low energy nuclear spin excitations in double perovskite compounds R$_2$CoMnO$_6$ (R = Y,Tb) by inelastic neutron scattering with a high-resolution back-scattering spectrometer. We observed inelastic signals at about 2.1 $\mu$eV for Y$_2$CoMnO$_6$ and also for Tb$_2$CoMnO$_6$ at T = 2 K in both energy loss and energy gain sides. We interpret these inelastic peaks to be due to the transitions between the hyperfine split nuclear levels of $^{59}$Co nucleus. The inelastic peaks move towards the central elastic peak and finally merge with it at the magnetic ordering temperature $T_C$. The energy of the low energy excitations decreases continuously and becomes zero at $T_C \approx 75$ K for Y$_2$CoMnO$_6$ and $T_C \approx 100$ K for Tb$_2$CoMnO$_6$. For Tb$_2$CoMnO$_6$, which contains magnetic rare-earth ions, additional quasielastic scattering due presumably to the fluctuations of large Tb magnetic moments was observed. The present study reveals the magnetic ordering of the Co sublattice. The results of this investigation along with that obtained by us for other compounds indicate the presence of unquenched orbital moments in some of the Co compounds.

We report the observation of spin glass state in the double perovskite oxide Sr$_{2}$FeCoO$_{6}$ prepared through sol-gel technique. Initial structural studies using x rays reveal that the compound crystallizes in tetragonal $I 4/m$ structure with lattice parameters, $a$ = 5.4609(2) \AA and $c$ = 7.7113(7) \AA. The temperature dependent powder x ray studies reveal no structural phase transition in the temperature range 10 -- 300 K. However, the unit cell volume shows an anomaly coinciding with the magnetic transition temperature thereby suggesting a close connection between lattice and magnetism. Neutron diffraction studies and subsequent bond valence sums analysis show that in Sr$_{2}$FeCoO$_{6}$, the $B$ site is randomly occupied by Fe and Co in the mixed valence states of Fe$^{3+}$/Fe$^{4+}$ and Co$^{3+}$/Co$^{4+}$. The random occupancy and mixed valence sets the stage for inhomogeneous magnetic exchange interactions and in turn, for the spin glass like state in this double perovskite which is observed as an irreversibility in temperature dependent dc magnetization at $T_f\sim$ 75 K. Thermal hysteresis observed in the magnetization profile of Sr$_{2}$FeCoO$_{6}$ is indicative of the mixed magnetic phases present. The dynamic magnetic susceptibility displays characteristic frequency dependence and confirms the spin glass nature of this material. Dynamical scaling analysis of $\chi'(T)$ yields a critical temperature $T_{ct}$ = 75.14(8) K and an exponent $z\nu$ = 6.2(2) typical for spin glasses. The signature of presence of mixed magnetic interactions is obtained from the thermal hysteresis in magnetization of Sr$_{2}$FeCoO$_{6}$. Combining the neutron and magnetization results of Sr$_2$FeCoO$_6$, we deduce the spin states of Fe to be in low spin while that of Co to be in low spin and intermediate spin., Comment: 23 pages, 6 figures, accepted in J. Appl. Phys

The Griffiths phase-like features and the spin-phonon coupling effects observed in Tb$_2$NiMnO$_6$ are reported. The double perovskite compound crystallizes in monoclinic $P2_1/n$ space group and exhibits a magnetic phase transition at $T_c \sim$ 111 K as an abrupt change in magnetization. A negative deviation from ideal Curie-Weiss law exhibited by 1/$\chi(T)$ curves and less-than-unity susceptibility exponents from the power-law analysis of inverse susceptibility are reminiscent of Griffiths phase-like features. Arrott plots derived from magnetization isotherms support the inhomogeneous nature of magnetism in this material. The observed effects originate from antiferromagnetic interactions which arise from inherent disorder in the system. Raman scattering experiments display no magnetic-order-induced phonon renormalization below $T_c$ in Tb$_2$NiMnO$_6$ which is different from the results observed in other double perovskites and is correlated to the smaller size of the rare earth. The temperature evolution of full-width-at-half-maximum for the {\it stretching} mode at 645 cm$^{-1}$ presents an anomaly which coincides with the magnetic transition temperature and signals a close connection between magnetism and lattice in this material., Comment: 17 pages, 8 figures; accepted in J. Appl. Phys

Hexagonal Dy(0.5)Y(0.5)MnO3, a multiferroic rare-earth manganite with geometrically frustrated antiferromagnetism, has been investigated with single-crystal neutron diffraction measurements. Below 3.4 K magnetic order is observed on both the Mn (antiferromagnetic) and Dy (ferrimagnetic) sublattices that is identical to that of undiluted hexagonal DyMnO3 at low temperature. The Mn moments undergo a spin reorientation transition between 3.4 K and 10 K, with antiferromagnetic order of the Mn sublattice persisting up to 70 K; the antiferromagnetic order in this phase is distinct from that observed in undiluted (h)DyMnO3, yielding a qualitatively new phase diagram not seen in other hexagonal rare-earth manganites. A magnetic field applied parallel to the crystallographic c axis will drive a transition from the antiferromagnetic phase into the low-temperature ferrimagnetic phase with little hysteresis., Comment: Six pages, four figures v2: Table I added, Figures 2 and 3 edited, text edited. August 24, 2011