arXiv subjects

A. A. Belik

Publications and source records attributed to A. A. Belik.

At least 19 recordsLinked to original sources

arXiv2024

Polarity vs Chirality: Functionality from competing magneto-structural instabilities

We report a phenomenological magneto-structural model based on competing free-energy terms that couple either polar or chiral distortions in cubic quadruple perovskites, depending on the global direction of magnetic moments. The model naturally explains why some compounds in this material system host magnetically-induced ferroelectricity at low temperature, while others such as CaMn$_3$(Cr$_3$Mn)O$_{12}$, which we characterise experimentally, do not. Importantly, our results suggest a new approach towards developing an applied multiferroic functionality, and can be generalised to other multi-sublattice systems where the magnetic interaction between sublattices is prohibited by spatial inversion.

cond-mat.mtrl-sci↗

arXiv2024

Two Displacive Ferroelectric Phase Transitions in Multiferroic Quadruple Perovskite $BiMn_{7}O_{12}$

We report on the microwave, terahertz (THz), infrared and Raman spectroscopic studies of $BiMn_{7}O_{12}$ ceramics, shedding more light into the nature of two structural phase transitions and their possible relation with ferroelectricity in this compound. We observed a softening of one polar phonon in the THz range on cooling towards 460 and 300 K, i.e., temperatures at which $BiMn_{7}O_{12}$ undergoes subsequent structural phase transitions from monoclinic $\textit{I2/m}$ to polar monoclinic $\textit{Im}$ and triclinic $\textit{P1}$ phases. The soft phonon causes dielectric anomalies typical for displacive ferroelectric phase transitions. Microwave measurements performed at 5.8 GHz up to 400 K qualitatively confirmed not only the dielectric anomaly at 300 K, but also revealed two other weak dielectric anomalies near the magnetic phase transitions at 60 K and 28 K. This evidences the multiferroic nature of the low-temperature phases, although the relatively high conductivity in the kHz and Hz spectral range prevented us from directly measuring the permittivity and ferroelectric polarization. Some Raman modes sense the magnetic phase transitions occurring near 60 and 25 K, showing that spin-phonon coupling is relevant in this compound and in this temperature range. The deviation of the Mn-O stretching mode frequency from the anharmonic temperature behavior was successfully explained by the spin correlation function calculated from the magnetic contribution to the specific heat.

cond-mat.mtrl-sci↗

arXiv2023

Magnetic inhomogeneities in the quadruple perovskite manganite [Y$_{2-x}$Mn$_x$]MnMnMn$_4$O$_{12}$

A combination of competing exchange interactions and substitutional disorder gives rise to magnetic inhomogeneities in the [Y$_{2-x}$Mn$_x$]MnMnMn$_4$O$_{12}$ $x = 0.23$ and $x = 0.16$ quadruple perovskite manganites. Our neutron powder scattering measurements show that both the $x = 0.23$ and $x = 0.16$ samples separate into two distinct magnetic phases; below T$_{1}$ = 120 $\pm$ 10 K the system undergoes a transition from a paramagnetic phase to a phase characterised by short range antiferromagnetic clusters contained in a paramagnetic matrix, and below T$_{2}$ $\sim$ 65 K, the system is composed of well correlated long range collinear ferrimagnetic order, punctuated by short range antiferromagnetic clusters. A sharp increase in the antiferromagnetic phase fraction is observed below $\sim$ 33 K, concomitant with a decrease in the ferrimagnetic phase fraction. Our results demonstrate that the theoretically proposed AFM phase is stabilised in the [Y$_{2-x}$Mn$_x$]MnMnMn$_4$O$_{12}$ manganites in the presence of dominant B-B exchange interactions, as predicted.

cond-mat.str-el↗

arXiv2021

Competing electronic instabilities in the quadruple perovskite manganite PbMn$_{7}$O$_{12}$

Structural behaviour of PbMn$_{7}$O$_{12}$ has been studied by high resolution synchrotron X-ray powder diffraction. This material belongs to a family of quadruple perovskite manganites that exhibit an incommensurate structural modulation associated with an orbital density wave. It has been found that the structural modulation in PbMn$_{7}$O$_{12}$ onsets at 294 K with the incommensurate propagation vector $\mathbf{k}_s=(0,0,\sim2.08)$. At 110 K another structural transition takes place where the propagation vector suddenly drops down to a \emph{quasi}-commensurate value $\mathbf{k}_s=(0,0,2.0060(6))$. The \emph{quasi}-commensurate phase is stable in the temperature range of 40K - 110 K, and below 40 K the propagation vector jumps back to the incommensurate value $\mathbf{k}_s=(0,0,\sim2.06)$. Both low temperature structural transitions are strongly first order with large thermal hysteresis. The orbital density wave in the \emph{quasi}-commensurate phase has been found to be substantially suppressed in comparison with the incommensurate phases, which naturally explains unusual magnetic behaviour recently reported for this perovskite. Analysis of the refined structural parameters revealed that that the presence of the \emph{quasi}-commensurate phase is likely to be associated with a competition between the Pb$^{2+}$ lone electron pair and Mn$^{3+}$ Jahn-Teller instabilities.

cond-mat.str-el↗

arXiv2020

Structural stability of CuAl$_{2}$O$_{4}$ under pressure

Structural properties of CuAl$_{2}$O$_{4}$, which was recently argued to show unusual suppression of the Jahn-Teller distortions by the spin-orbit coupling, are investigated under pressures up to 6 GPa. Analysis of X-ray powder diffraction experiments shows that CuAl$_{2}$O$_{4}$ gets unstable and decomposes onto CuO and Al$_{2}$O$_{3}$ at pressures $\sim$ 6 GPa and temperature $\sim$ 1000 K. This finding is complemented by the DFT+U+SOC calculations, which demonstrate that this instability is partially driven by a (relatively) large compressibility of strongly Jahn-Teller distorted CuO.

cond-mat.str-el↗

arXiv2020

Spontaneous Rotation of Ferrimagnetism Driven by Antiferromagnetic Spin Canting

Spin-reorientation phase transitions that involve the rotation of a crystal$'$s magnetization have been well characterized in distorted-perovskite oxides such as the orthoferrites. In these systems spin reorientation occurs due to competing rare-earth and transition metal anisotropies coupled via $f$-$d$ exchange. Here, we demonstrate an alternative paradigm for spin reorientation in distorted perovskites. We show that the $R_2\mathrm{CuMnMn_4O_{12}}$ (R = Y or Dy) triple A-site columnar-ordered quadruple perovskites have three ordered magnetic phases and up to two spin-reorientation phase transitions. Unlike the spin-reorientation phenomena in other distorted perovskites, these transitions are independent of rare-earth magnetism, but are instead driven by an instability towards antiferromagnetic spin canting likely originating in frustrated Heisenberg exchange interactions, and the competition between Dzyaloshinskii-Moriya and single-ion anisotropies.

cond-mat.str-el↗

arXiv2019

The magnetic structure and spin-flop transition in the A-site columnar-ordered quadruple perovskite $\mathrm{TmMn_3O_6}$

We present the magnetic structure of $\mathrm{TmMn_3O_6}$, solved via neutron powder diffraction - the first such study of any $R\mathrm{Mn_3O_6}$ A-site columnar-ordered quadruple perovskite to be reported. We demonstrate that long range magnetic order develops below 74 K, and at 28 K a spin-flop transition occurs driven by $f$-$d$ exchange and rare earth single ion anisotropy. In both magnetic phases the magnetic structure may be described as a collinear ferrimagnet, contrary to conventional theories of magnetic order in the manganite perovskites. Instead, we show that these magnetic structures can be understood to arise due to ferro-orbital order, the A, A$'$ and A$''$ site point symmetry, $mm2$, and the dominance of A-B exchange over both A-A and B-B exchange, which together are unique to the $R\mathrm{Mn_3O_6}$ perovskites.

cond-mat.str-el↗

arXiv2018

The magnetic structures of rare-earth quadruple perovskite manganites $R$Mn$_7$O$_{12}$

We report a neutron powder diffraction study of $R$Mn$_7$O$_{12}$ quadruple perovskite manganites with $R$ = La, Ce, Nd, Sm, and Eu. We show that in all measured compounds concomitant magnetic ordering of the $A$ and $B$ manganese sublattices occurs on cooling below the N$\mathrm{\acute{e}}$el temperature. The respective magnetic structures are collinear, with one uncompensated Mn$^{3+}$ moment per formula unit as observed in bulk magnetisation measurements. We show that both LaMn$_7$O$_{12}$ and NdMn$_7$O$_{12}$ undergo a second magnetic phase transition at low temperature, which introduces a canting of the $B$ site sublattice moments that is commensurate in LaMn$_7$O$_{12}$ and incommensurate in NdMn$_7$O$_{12}$. This spin canting is consistent with a magnetic instability originating in the $B$ site orbital order. Furthermore, NdMn$_7$O$_{12}$ displays a third magnetic phase transition at which long range ordering of the Nd sublattice modifies the periodicity of the incommensurate spin canting. Our results demonstrate a rich interplay between transition metal magnetism, orbital order, and the crystal lattice, which may be fine tuned by cation substitution and rare earth magnetism.

cond-mat.str-el↗

arXiv2017

Universal magneto-orbital ordering in the divalent $A$-site quadruple perovskite manganites $A$Mn$_7$O$_{12}$ ($A$ = Ca, Sr, Cd, and Pb)

Through analysis of variable temperature neutron powder diffraction data, we present solutions for the magnetic structures of SrMn$_7$O$_{12}$, CdMn$_7$O$_{12}$, and PbMn$_7$O$_{12}$ in all long-range ordered phases. The three compounds were found to have magnetic structures analogous to that reported for CaMn$_7$O$_{12}$. They all feature a higher temperature lock-in phase with \emph{commensurate} magneto-orbital coupling, and a delocked, multi-\textbf{k} magnetic ground state where \emph{incommensurate} magneto-orbital coupling gives rise to a constant-moment magnetic helix with modulated spin helicity. CdMn$_7$O$_{12}$ represents a special case in which the orbital modulation is commensurate with the crystal lattice and involves stacking of fully and partially polarized orbital states. Our results provide a robust confirmation of the phenomenological model for magneto-orbital coupling previously presented for CaMn$_7$O$_{12}$. Furthermore, we show that the model is universal to the $A^{2+}$ quadruple perovskite manganites synthesised to date, and that it is tunable by selection of the $A$-site ionic radius.

cond-mat.str-el↗

arXiv2015

Magnetic excitations from an S=1/2 diamond-shaped tetramer compound Cu2PO4OH

Inelastic neutron scattering experiments have been carried out on a powder sample of Cu2PO4OH, which consists of diamond-shaped tetramer spin units with S=1/2. We have observed two nearly dispersionless magnetic excitations at E1~12 and E2~20 meV, whose energy width are broader than the instrumental resolution. The simplest square tetramer model with one dominant interaction, which predicts two sharp excitation peaks at E1 and E2(=2E1), does not explain the experimental result. We found that two diagonal intratetramer interactions compete with the main interaction and weak intertetramer interactions connect the tetramers. The main intratetramer interaction is found to split into two inequivalent ones due to a structural distortion below 160 K. Cu2PO4OH is considered to be a good material to study the S=1/2 Heisenberg tetramer system.

cond-mat.mtrl-sci↗

arXiv2014

Strong spin-phonon coupling in infrared and Raman spectra of SrMnO3

Infrared reflectivity spectra of cubic SrMnO$_{3}$ ceramics reveal 18 % stiffening of the lowest-frequency phonon below the antiferromagnetic phase transition occurring at T$_{N}$ = 233 K. Such a large temperature change of the polar phonon frequency is extraordinary and we attribute it to an exceptionally strong spin-phonon coupling in this material. This is consistent with our prediction from first principles calculations. Moreover, polar phonons become Raman active below T$_{N}$, although their activation is forbidden by symmetry in $Pm\bar{3}m$ space group. This gives evidence that the cubic $Pm\bar{3}m$ symmetry is locally broken below T$_{N}$ due to a strong magnetoelectric coupling. Multiphonon and multimagnon scattering is also observed in Raman spectra. Microwave and THz permittivity is strongly influenced by hopping electronic conductivity, which is caused by small non-stoichiometry of the sample. Thermoelectric measurements show room-temperature concentration of free carriers $n_{e}=$3.6 10$^{20}$ cm$^{-3}$ and the sample composition Sr$^{2+}$Mn$_{0.98}^{4+}$Mn$_{0.02}^{3+}$O$_{2.99}^{2-}$. The conductivity exhibits very unusual temperature behavior: THz conductivity increases on cooling, while the static conductivity markedly decreases on cooling. We attribute this to different conductivity of the ceramic grains and grain boundaries.

cond-mat.mtrl-sci↗

arXiv2012

Absence of ferroelectricity in BiMnO3 ceramics

We performed factor-group analysis of all phonons in possible monoclinic C2/c and C2 structures of BiMnO3 and compared it with our experimental infrared and Raman spectra. We conclude that the crystal structure is centrosymmetric C2/c in the whole investigated temperature range from 10 to 550 K, therefore BiMnO3 cannot be ferroelectric. We revealed a dielectric relaxation in THz spectra above the structural phase transition taking place at T_C1=475 K giving evidence in strong lattice anharmonicity and a large dynamical disorder of Bi cations above T_C1. Step-like dielectric anomaly observed at T_C1 in THz permittivity reminds antiferroelectric phase transition. Nevertheless, the low-temperature dielectric studies did not reveal any antiferroelectric or ferroelectric hysteresis loop. Our experimental results support theoretical paper of P. Baettig et al. (J. Am. Chem. Soc. 129, 9854 (2007)) claiming that BiMnO3 is not multiferroic, but only antipolar ferromagnet.

cond-mat.mtrl-sci↗

arXiv2012

Antiferrodistortive phase transition in EuTiO3

X-ray diffraction, dynamical mechanical analysis and infrared reflectivity studies revealed an antiferrodistortive phase transition in EuTiO3 ceramics. Near 300K the perovskite structure changes from cubic Pm-3m to tetragonal I4/mcm due to antiphase tilting of oxygen octahedra along the c axis (a0a0c- in Glazer notation). The phase transition is analogous to SrTiO3. However, some ceramics as well as single crystals of EuTiO3 show different infrared reflectivity spectra bringing evidence of a different crystal structure. In such samples electron diffraction revealed an incommensurate tetragonal structure with modulation wavevector q ~ 0.38 a*. Extra phonons in samples with modulated structure are activated in the IR spectra due to folding of the Brillouin zone. We propose that defects like Eu3+ and oxygen vacancies strongly influence the temperature of the phase transition to antiferrodistortive phase as well as the tendency to incommensurate modulation in EuTiO3.

cond-mat.mtrl-sci↗

arXiv2011

InMnO3 : a fully frustrated multiferroic

InMnO$_3$ is a peculiar member of the hexagonal manganites h-RMnO$_3$ (where R is a rare earth metal element), showing crystalline, electronic and magnetic properties at variance with the other compounds of the family. We have studied high quality samples synthesized at high pressure and temperature by powder neutron diffraction. The position of the Mn ions is found to be close to the threshold $\it{x}=1/3$ where superexchange Mn-Mn interactions along the $\it{c}$ axis compensate. Magnetic long range order occurs below $T_{\rm N}$= 120(2) K with a magnetic unit cell doubled along $\it{c}$, whereas short range two dimensional dynamical spin correlations are observed above $T_{\rm N}$. We propose that pseudo-dipolar interactions are responsible for the long period magnetic structure.

cond-mat.mtrl-sci↗

arXiv2010

Large decrease in the critical temperature of superconducting LaFeAsO0.85 compounds doped with 3% atomic weight of nonmagnetic Zn impurities

We observed a large decrease of Tc by no more than 3 at.% of Zn doped to the optimized superconductor LaFeAsO0.85 (Tc = 26 K), confirmed by measurements of electrical resistivity, magnetic susceptibility, specific heat, Mössbauer spectroscopy, Hall coefficient, and an electron probe micro-analysis. The rate ~9 K/% is remarkably higher than observations regarding nonmagnetic impurities. The Tc suppression is likely due to pair-breaking caused by scatterings associated with highly localized electronic state of Zn doped into the Fe2As2 layer. If this is true, the Zn result well accords with the theoretical prediction that suggests a sign reversal s-wave pairing model for the Fe pnictide superconductors, unlike other nonmagnetic impurity results.

cond-mat.supr-con↗

arXiv2010

Anomalous pressure effect on the magnetic ordering in multiferroic BiMnO3

We report the magnetic field dependent dc magnetization and the pressure-dependent (pmax ~ 16 kbar) ac susceptibilities Xp(T) on both powder and bulk multiferroic BiMnO3 samples, synthesized in different batches under high pressure. A clear ferromagnetic (FM) transition is observed at TC ~ 100 K, and increases with magnetic field. The magnetic hysteresis behavior is similar to that of a soft ferromagnet. Ac susceptibility data indicate that both the FM peak and its temperature (TC) decrease simultaneously with increasing pressure. Interestingly, above a certain pressure (9 ~ 11 kbar), another peak appears at Tp ~ 93 K, which also decreases with increasing pressure, with both these peaks persisting over some intermediate pressure range (9 ~ 13 kbar). The FM peak disappears with further application of pressure; however, the second peak survives until present pressure limit (pmax ~ 16 kbar). These features are considered to originate from the complex interplay of the magnetic and orbital structure of BiMnO3 being affected by pressure.

cond-mat.str-el↗

arXiv2010

Multiple magnetic transitions in multiferroic BiMnO3

The magnetic phase variations under hydrostatic pressure on multiferroic BiMnO3 have been examined by the dc magnetization [Mg(T)], magnetic hysteresis [Ueff(H)], and ac susceptibility [X'g(T)]. Three magnetic transitions, manifested as kinks I, II, and III on the Mg(T)], curves, were identified at 8.7 and 9.4 kbar. With increasing pressure, transition temperatures of kink I and kink II TkI and TkII tend to decrease, but the temperature of kink III TkIII showed more complex variation. Under increasing magnetic field, TkI and TkII increase; however, TkIII decreases. Combining [Mg(T)] curves with Ueff(H) and X'g(T), more detailed properties of these three kinks would be shown as follows. Kink I is a long-range soft ferromagnetic transition which occurs at TkI 100 K under ambient pressure but is suppressed completely at 11.9 kbar. Kink II emerges at 8.7 kbar along with TkII 93 K which is also long-range soft ferromagnetic but canted in nature. Kink III, a canted antiferromagnetic transition, appears at TkIII 72.5 K along with kink II also at 8.7 kbar. The proposed phase diagrams at ambient pressure, 9.4 and 11.9 kbar show the different magnetic features of BiMnO3. These findings are believed to result from the variations in crystal structure influenced by the external pressure. These results also indicate the common complicated

cond-mat.str-el↗

arXiv2009

Drastic suppression of the superconductivity of LaFeAsO0.85 by a nonmagnetic impurity

We observed a drastic Tc suppression caused by no more than 3 at.% of Zn doped to the optimized superconductor LaFeAsO0.85 (Tc = 26 K). The electrical resistivity and magnetic susceptibility measurements suggested that it is likely due to impurity scatterings rather than losing the metallic nature, seeming to support the s+/- pairing model proposed for the Fe pnictide superconductor.

cond-mat.supr-con↗