arXiv subjects

Alexei A. Belik

Publications and source records attributed to Alexei A. Belik.

18 recordsLinked to original sources

arXiv2026

Quasi two dimensional magnetic structure of the triclinic double perovskite Ca$_2$CuWO$_6$

We present the antiferromagnetic ground state of the triclinic double perovskite Ca$_2$CuWO$_6$solved by neutron powder diffraction, and analyze it in direct comparison with tetragonal Sr$_2$CuWO$_6$. Below $T_\mathrm{N} \simeq 32$ K, the magnetic Bragg reflections of Ca$_2$CuWO$_6$ are indexed by the commensurate propagation vector $\mathbf{k}=(\tfrac{1}{2},\tfrac{1}{2},0)$ in its native $P\bar{1}$ cell. Rietveld refinement yields a collinear structure with equal-magnitude, antiparallel moments on the crystallographically inequivalent Cu1 and Cu2 sites and an ordered moment of $0.66(3)~μ_{\mathrm B}$ per Cu at 1.5 K. A direct comparison with Sr$_2$CuWO$_6$ is obscured by different crystallographic settings and orientations of the cooperative Jahn-Teller elongation axes. Hence, we introduce a common crystallographic supercell through which effects of symmetry lowering from tetragonal to triclinic in the double perovskite are explored: Apparently different magnetic propagation vectors map onto the same supercell wave vector, revealing a common magnetic structure stabilized by tungsten-mediated, second-neighbor interactions. Mean field calculations further show that tetragonal symmetry preserves the degeneracy of four magnetic $\mathbf{k}$-domains in Sr$_2$CuWO$_6$, whereas the triclinic splitting of symmetry-related exchange pathways in Ca$_2$CuWO$_6$, most strongly within the Cu2 network, selects a single $\mathbf{k}$-domain. These results establish the magnetic ground state of Ca$_2$CuWO$_6$ and show how symmetry breaking selects a given ordered state without changing the underlying magnetic motif of the Sr analogue.

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arXiv2026

Inverse Melting of 3D Antiferromagnetic Order in Multi-sublattice Magnetic Perovskites

In conventional antiferromagnets a long-range ordered 3D ground state transitions to a disordered paramagnetic state on warming, often via lower dimensional spin correlations within the critical regime. Here we demonstrate a striking departure from this paradigm. Through analysis of neutron powder diffraction data, we show that the magnetic ground state of columnar-ordered quadruple perovskites, Na$R$Mn$_2$Ti$_4$O$_{12}$ ($R$ = Dy, Sm), lacks long-range order, hosting only 2D spin correlations. On warming, this disordered state transitions into a 3D long-range ordered antiferromagnetic structure prior to the phase transition to the paramagnetic state. Our results establish an unconventional order-by-heating mechanism in which intrinsic A-site chemical disorder is coupled to competing exchange interactions between the rare earth and Mn sub-lattices, leading to a novel type of magnetic phase transition.

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arXiv2026

Magnetic behavior of the $5d^1$ Re-based double perovskite Sr$_2$ZnReO$_6$

The subtle interplay between spin-orbit coupling, exchange interactions, and cation ordering can lead to exotic magnetic states in transition-metal ions. We report a comprehensive study of the Re-based (5$d^1$) ordered double perovskite oxide Sr$_2$ZnReO$_6$ combining synchrotron x-ray diffraction (XRD), magnetic susceptibility, muon spin relaxation ($μ$SR) measurements, and density functional theory (DFT) calculations. XRD reveals that Sr$_2$ZnReO$_6$ crystallizes in the monoclinic structure (space group $P2_1/n$) at low temperature. Magnetic susceptibility data indicate a transition below $\sim$13 K, with $M$--$H$ loops showing ferromagnetic-like hysteresis and an unusually high coercive field of 23 kOe at 2 K. Zero-field $μ$SR measurements detect static and spatially disordered internal fields below $T_M \simeq $ 12 K, consistent with a canted antiferromagnetic ground state determined by detailed DFT and force-theorem in Hubbard-I calculations. The reduced high-temperature effective moment ($\sim0.76~μ_B$) and very small static moment ($\lesssim 0.2~μ_B$) derived from $μ$SR analysis and local-field simulations indicate a decisive role of spin-orbit coupling. Through a combined experimental and computational approach we unambiguously determine the canted antiferromagnetic order in Sr$_2$ZnReO$_6$, showing that a very small ordered moment coexists with an exceptionally large coercivity. These results underscore the crucial role of spin-orbit coupling and orbital ordering, providing new insights into magnetism in 5$d^1$ double perovskites.

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arXiv2026

Dielectric, magnetic and lattice dynamics properties of double perovskite (Ca0.5Mn1.5)MnWO6

Recent dielectric and magnetic studies of (Ca0.5Mn1.5)MnWO6 ceramics [A.A. Belik, Chem. Mater. 36, 7604 (2024)] have classified this material as a rare hybrid multiferroic, with both antiferromagnetic and (anti)ferroelectric ordering occurring at the same temperature of 22 K. The pronounced dielectric anomaly observed at this temperature indicated that the structural change is primarily induced by a phonon soft mode and not by a spin arrangement, as is usually the case in type II multiferroics. However, our comprehensive investigation involving new ceramic samples as well as the sample from the above-mentioned reference does not support this conclusion. Low-temperature polarization measurements revealed no evidence of either ferroelectric or antiferroelectric order in both sample series. The dielectric permittivity exhibits only a slight change at the antiferromagnetic transition, and phonon modes observed in IR and Raman spectra show no indication of a symmetry change at low temperatures. In the new samples the Neel temperature is shifted to TN = 18 K. XRD, SEM, EDS and WDS analyses confirmed the composition (Ca0.5Mn1.5)MnWO6 of both ceramics, but also indicated a small amount (percentage points) of MnO and CaO impurities in the sample from the previous publication and Mn3O4, CaWO4 secondary phases (<4%) in the new ceramics. The differences in dielectric and magnetic properties of the two samples can therefore be explained by their different chemical purity. The small dielectric anomaly of the new sample at the antiferromagnetic transition temperature is explained by a spin-phonon coupling. We conclude that (Ca0.5Mn1.5)MnWO6 is not a multiferroic, but a paraelectric antiferromagnet.

cond-mat.mtrl-sci↗

arXiv2024

Exotic magnetism in perovskite KOsO3

A new perovskite KOsO3 has been stabilized under high-pressure and high temperature conditions. It is cubic at 500 K (Pm-3m) and undergoes subsequent phase transitions to tetragonal at 320 K (P4/mmm) and rhombohedral (R-3m) at 230 K as shown from refining synchrotron X-ray powder diffraction (SXRD) data. The larger orbital overlap integral and the extended wavefunction of 5d electrons in the perovskite KOsO3 allow to explore physics from the regime where Mott and Hund's rule couplings dominate to the state where the multiple interactions are on equal footing. We demonstrate an exotic magnetic ordering phase found by neutron powder diffraction along with physical properties via a suite of measurements including magnetic and transport properties, differential scanning calorimetry, and specific heat, which provide comprehensive information for a system at the crossover from localized to itinerant electronic behavior.

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arXiv2022

Can the Ferroelectric Soft Mode Trigger an Antiferromagnetic Phase Transition?

Type-II multiferroics, where spin interactions induce a ferroelectric polarization, are interesting for new device functionalities due to large magnetoelectric coupling. We report on a new type of multiferroicity in the quadruple-perovskite $\text{BiMn}_{\text{3}}\text{Cr}_{\text{4}}\text{O}_{\text{12}}$, where an antiferromagnetic phase is induced by the structural change at the ferroelectric phase transition. The displacive nature of the ferroelectric phase transition at 125 K, with a crossover to an order-disorder mechanism, is evidenced by a polar soft phonon in the THz range and a central mode. Dielectric and pyroelectric studies show that the ferroelectric critical temperature corresponds to the previously reported Néel temperature of the $\text{Cr}^{\text{3+}}$ spins. An increase in ferroelectric polarization is observed below 48 K, coinciding with the Néel temperature of the $\text{Mn}^{\text{3+}}$ spins. This increase in polarization is attributed to an enhanced magnetoelectric coupling, as no change in the crystal symmetry below 48 K is detected from infrared and Raman spectra.

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arXiv2020

Unusual effects of magnetic dilution in the ferrimagnetic columnar ordered $\mathrm{Sm_2MnMnMn_{4-x}Ti_xO_{12}}$ perovskites

Powder neutron diffraction experiments have been employed to establish the effects of site-selective magnetic dilution in the Sm2MnMnMn4-x Tix O12 A-site columnar ordered quadruple perovskite manganites (x = 1, x = 2 and x = 3). We show that in all three compositions the Mn ions adopt a collinear ferrimagnetic structure below 27 K, 62 K and 34 K, respectively. An unexpected increase in the ordering temperature was observed between the x = 1 and x = 2 samples, which indicates a considerable departure from mean field behaviour. This result is corroborated by large reductions in the theoretical ground state magnetic moments observed across the series, which indicate the presence of spin fluctuations and or disorder. We show that long range magnetic order in the x = 3 sample, which occurs below the percolation threshold for B-B exchange, can only be understood to arise if magnetic order in Sm2MnMnMn4-xTixO12 is mediated via both A-B and B-B exchange, hence confirming the importance of A-B exchange interactions in these materials. Finally we show that site-selective magnetic dilution enables the tuning of a ferrimagnetic compensation point and the introduction of temperature-induced magnetization reversal.

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arXiv2020

Emergent helical texture of electric dipoles

Long-range ordering of magnetic dipoles in bulk materials gives rise to a broad range of magnetic structures, from simple collinear ferromagnets and antiferromagnets, to complex magnetic helicoidal textures stabilized by competing exchange interactions. In contrast, in the context of dipolar order in dielectric crystals, only parallel (ferroelectric) and antiparallel (antiferroelectric) collinear alignments of electric dipoles are typically considered. Here, we report an observation of incommensurate helical ordering of electric dipoles by light hole-doping of the quadruple perovskite BiMn7O12. In analogy with magnetism, the electric dipole helicoidal texture is also stabilized by competing instabilities. Specifically, orbital ordering and lone electron pair stereochemical activity compete, giving rise to phase transitions from a non-chiral cubic structure, to an incommensurate electric dipole and orbital helix, via an intermediate density wave.

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arXiv2020

Study of polycrystalline bulk Sr$_3$OsO$_6$ double-perovskite insulator: comparison with 1000 K ferromagnetic epitaxial films

Polycrystalline Sr$_3$OsO$_6$, which is an ordered double-perovskite insulator, is synthesized via solid-state reaction under high-temperature and high-pressure conditions of 1200 $^\circ$C and 6 GPa. The synthesis enables us to conduct a comparative study of the bulk form of Sr$_3$OsO$_6$ toward revealing the driving mechanism of 1000 K ferromagnetism, which has recently been discovered for epitaxially grown Sr$_3$OsO$_6$ films. Unlike the film, the bulk is dominated by antiferromagnetism rather than ferromagnetism. Therefore, robust ferromagnetic order appears only when Sr$_3$OsO$_6$ is under the influence of interfaces. A specific heat capacity of 39.6(9) 10$^{-3}$ J mol$^{-1}$ K$^{-2}$ is found at low temperatures ($<$17 K). This value is remarkably high, suggesting the presence of possible fermionic-like excitations at the magnetic ground state. Although the bulk and film forms of Sr$_3$OsO$_6$ share the same lattice basis and electrically insulating state, the magnetism is entirely different between them.

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arXiv2019

Colossal magnetoresistance in the insulating ferromagnetic double perovskites Tl$_2$NiMnO$_6$: A neutron diffraction study

In the family of double perovskites, colossal magnetoresistance (CMR) has been so far observed only in half-metallic ferrimagnets such as the known case Sr$_2$FeMoO$_6$ where it has been assigned to the tunneling MR at grain boundaries due to the half-metallic nature. Here we report a new material-Tl$_2$NiMnO$_6$, a relatively ordered double perovskite stablized by the high pressure and high temperature synthesis-showing CMR in the vicinity of its Curie temperature. We explain the origin of such effect with neutron diffraction experiment and electronic structure calculations that reveal the material is a ferromagnetic insulator. Hence the ordered Tl$_2$NiMnO$_6$ (~70% of Ni$^{2+}$/Mn$^{4+}$ cation ordering) represents the first realization of a ferromagnetic insulating double perovskite, showing CMR. The study of the relationship between structure and magnetic properties allows us to clarify the nature of spin glass behaviour in the disordered Tl$_2$NiMnO$_6$ (~31% of cation ordering), which is related to the clustering of antisite defects and associated with the short-range spin correlations. Our results highlight the key role of the cation ordering in establishing the long range magnetic ground state and lay out new avenues to exploit advanced magnetic materials in double perovskites.

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arXiv2019

Spin and orbital ordering in TlMnO3: Neutron diffraction study

Crystal and magnetic structures of the high-pressure stabilized perovskite phase of TlMnO3 have been studied by neutron powder diffraction. The crystal structure involves two types of primary structural distortions: a+b-b-octahedral tilting and antiferrodistortive type of orbital ordering, whose common action reduces the symmetry down to triclinic P -1. The orbital pattern and the way it is combined with the octahedral tilting are different from the family of LnMnO3 (Ln = lanthanide or Y) manganites who share with TlMnO3 the same tilting scheme. The experimentally determined magnetic structure with the k = (1/2,0,1/2) propagation vector and P_S-1 symmetry implies anisotropic exchange interactions with a ferromagnetic coupling within the (1,0,-1) planes and an antiferromagnetic one between them (A type). The spins in the primary magnetic mode were found to be confined close to the (1,0,-1) plane, which underlines the predominant role of the single ion anisotropy with the local easy axes of Mn3+ following the Jahn-Teller distortions of the octahedra. In spite of the same octahedral tilting scheme in the perovskite structures of both LnMnO3 and TlMnO3 manganites, a coupling of the secondary ferromagnetic component to the primary A-type spin configuration through antisymmetric exchange interaction is allowed in the former and forbidden in the latter cases.

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arXiv2019

Magnetic ordering and ferroelectricity in multiferroic 2H-AgFeO2: Comparison between hexagonal and rhombohedral polytypes

Magnetic and dielectric properties of the hexagonal triangular lattice antiferromagnet 2H-AgFeO2 have been studied by neutron diffraction, magnetic susceptibility, specific heat, pyroelectric current, and dielectric constant measurements. The ferroelectric polarization, P ~ 5 μC/m2, has been found to appear below 11 K due to a polar nature of the magnetic ground state of the system. In the temperature range of 11 K < T < 18 K, an incommensurate spin density wave (ICM1) with the nonpolar magnetic point group mmm1' and the k1 = (0,q1_b,0; q1_b = 0.390-0.405)propagation vector takes place. Below 14 K, a proper screw ordering (ICM2) and k2 = (0,q2_b,0; q2_b = 0.385-0.396) appears as a minor phase which coexists with ICM1 and the ground state down to the lowestmeasured temperature 5.5 K. No ferroelectric polarization associated with the ICM2 phase was observed in agreement with its nonpolar point group 2221'. Finally, a spiral order with cycloid and proper screw components (ICM3), and k3 = (q3_a,q3_b,0; q3_a = 0.0467, q3_b = 0.349) emerges below 11 K as the ground state of the system. Based on the deduced magnetic point group 21', we conclude that the ferroelectric polarization in ICM3 is parallel to the c axis and is caused by the inverse Dzyloshinskii-Moriya effect with p1 ~ rij x (Si x Sj ). Unlike the rhombohedral 3R-AgFeO2 polytype, the additional contribution to the macroscopic polarization p2 ~ Si x Sj is not allowed in the present case due to the symmetry constraints imposed by the hexagonal lattice of 2H-AgFeO2.

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arXiv2019

Ferroelectricity induced by ferriaxial crystal rotation and spin helicity in a B-site-ordered double-perovskite multiferroic In2NiMnO6

We have performed dielectric measurements and neutron diffraction experiments on the double perovskite In2NiMnO6. A ferroelectric polarization, P ~ 30 μC/m2, is observed in a polycrystalline sample below TN = 26 K where a magnetic phase ransition occurs. The neutron diffraction experiment demonstrates that a complex noncollinear magnetic structure with "cycloidal" and "proper screw" components appears below TN, which has the incommensurate propagation vector k = (ka,0,ks; ka ~ 0.274, ks ~ -0.0893). The established magnetic point group 21' implies that the macroscopic ferroelectric polarization is along the monoclinic b axis. Recent theories based on the inverse Dzyaloshinskii-Moriya effect allow us to specify two distinct contributions to the polarization of In2NiMnO6. One of them is associated with the cycloidal component, p1 ~ rij x (Si x Sj), and the other with the proper screw component, p2 ~ [rij (Si x Sj )]A. The latter is explained by coupling between spin helicity and "ferriaxial" crystal rotation with macroscopic ferroaxial vector A, characteristic of the B-site ordered perovskite systems with out-of-plane octahedral tilting.

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arXiv2017

Unusual magnetic structure of high-pressure synthesized perovskites ACrO3(A=Sc, In, Tl)

Magnetic structures of metastable perovskites ScCrO3, InCrO3 and TlCrO3, stabilized under high-pressure and high-temperature conditions, have been studied by neutron powder diffraction. Similar to the other orthochromites LnCrO3 (Ln=lanthanide or Y), these materials crystallize into the orthorhombic structure with Pnma10 symmetry. The spin configuration of the metastable perovskites has been found to be C-type, contrasting with the G-type structure usually observed in LnCrO3. First-principles calculations demonstrate that the Ctype structure found in ScCrO3 and InCrO3 is attributed to a ferromagnetic (FM) nearest-neighbor interaction, while in TlCrO3, this type of magnetic ordering is stabilized by a strong next-nearest-neighbor antiferromagnetic (AFM) exchange. The spins in the C-type magnetic structure line up along the orthorhombic b-axis, yielding the Pnma magnetic symmetry. The dominant mechanism controlling this spin direction has been concluded to be the single ion anisotropy imposed by a uniaxial distortion of CrO6 octahedra.

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arXiv2017

57Fe Mössbauer study of unusual magnetic structure of multiferroic 3R-AgFeO2

We report new results of a 57Fe Mössbauer study of multiferroic 3R-AgFeO2 powder samples performed in a wide temperature range, including two points, TN1 ~ 14 K and TN2 ~ 9 K, of magnetic phase transitions. At the intermediate temperature range, TN2 < T < TN1, the 57Fe Mössbauer spectra can be described in terms of collinear spin-density-waves (SDW) with the inclusion of many high-order harmonics, indicating that the real magnetic structure of this ferrite appears to be more complicated than a pure sinusoidally modulated SDW. The spectra at low temperatures, T < TN2, consist of a Zeeman pattern with line broadenings and sizeable spectral asymmetry. It has been shown that the observed spectral shape is consistent with a transition to the elliptical cycloidal magnetic structure. An analysis of the experimental spectra was carried out under the assumption that the electric hyperfine interactions are modulated when the Fe3+ magnetic moment rotates with respect to the principal axis of the EFG tensor and emergence of the strong anisotropy of the magnetic hyperfine field Hhf at the 57Fe nuclei. The large and temperature-independent anharmonicity parameter, m ~ 0.78, of the cycloidal spin structure obtained from the experimental spectra results from easy-axis anisotropy in the plane of rotation of the iron spin. Analysis of different mechanisms of spin and hyperfine interactions in 3R-AgFeO2 and its structural analogue CuFeO2 points to a specific role played by the topology of the exchange coupling and the oxygen polarization in the delafossite structures.

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arXiv2012

Observation of persistent centrosymmetricity in the hexagonal manganite family

The controversy regarding the ferroelectric behavior of hexagonal InMnO$_3$ is resolved by using a combination of x-ray diffraction (XRD), piezoresponse force microscopy (PFM), second harmonic generation (SHG), and density functional theory (DFT). While XRD data show a symmetry-lowering unit-cell tripling, which is also found in the multiferroic hexagonal manganites of $P6_3cm$ symmetry, PFM and SHG do not detect ferroelectricity at ambient or low temperature, in striking contrast to the behavior in the multiferroic counterparts. We propose instead a centrosymmetric $P\bar{3}c$ phase as the ground state structure. Our DFT calculations reveal that the relative energy of the ferroelectric and nonferroelectric structures is determined by a competition between electrostatics and oxygen-$R$-site covalency, with an absence of covalency favoring the ferroelectric phase.

cond-mat.mtrl-sci↗

arXiv2008

Frustrated spin-1/2 square lattice in the layered perovskite PbVO(3)

We report on the magnetic properties of the layered perovskite PbVO(3). The results of magnetic susceptibility and specific heat measurements as well as band structure calculations consistently suggest that the S=1/2 square lattice of vanadium atoms in PbVO(3) is strongly frustrated due to next-nearest-neighbor antiferromagnetic interactions. The ratio of next-nearest-neighbor (J(2)) to nearest-neighbor (J(1)) exchange integrals is estimated to be J(2)/J(1)\approx 0.2-0.4. Thus, PbVO(3) is within or close to the critical region of the J(1)-J(2) frustrated square lattice. Supporting this, no sign of long-range magnetic ordering was found down to 1.8 K.

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arXiv2005

Local Electronic Structure of PbVO3, a New Member of PbTiO3 Family, studied by XANES/ELNES

Recently an interesting multi-ferroic system PbVO3 [Chem. Mater. 2004] was successfully prepared using a high-pressure and high-temperature technique. The crystallographic features were reported. In this note we concentrate on the theoretical XANES spectra by considering the K-edge of Vanadium. The tetragonality [c/a=1.229 at 300 K] of PbVO3 is the largest in the PbTiO3 family of compounds. Thus one is led naturally to examine the effect of the change of tetragonality and the axial oxygen position on the electronic structure [i.e. XANES spectrum]. We study this effect in two ways. At a given temperature we vary the tetragonality and the axial oxygen position and quantify it in terms of XANES difference spectrum. Secondly, we compute the XANES spectra at three different temperatures, 90 K, 300 K, and 530 K and quantify the change in terms of the difference spectrum. We note that in this compound the tetragonality increases almost monotonically with temperature from 12 K to 570 K without transition to the cubic phase under ambient pressure. A key objective of the current investigation is to gain an understanding of various absorption features in the vicinity of K-edge of V, in terms of valence, local site symmetry, local coordination geometry, local bond distances, charge transfer, and local projected density of states. We consider both the polarized and the unpolarized XANES spectra. In short we have performed a local electronic study, which nicely complements the crystallographic features reported recently in PbVO3.

cond-mat.mtrl-sci↗