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V. Tsurkan

Publications and source records attributed to V. Tsurkan.

At least 109 records · Page 6Linked to original sources

Evolution of magnetic states in frustrated diamond lattice antiferromagnetic Co(Al1-xCox)2O4 spinels

Using neutron powder diffraction and Monte-Carlo simulations we show that a spin-liquid regime emerges at $all compositions in the diamond-lattice antiferromagnets Co(Al1-xCox)2O4. This spin-liquid regime induced by frustration due to the second-neighbour exchange coupling J2, is gradually superseded by antiferromagnetic collinear long-range order (k=0) at low temperatures. Upon substitution of Al3+ by Co3+ in the octahedral B-site the temperature range occupied by the spin-liquid regime narrows and TN increases. To explain the experimental observations we considered magnetic anisotropy D or third-neighbour exchange coupling J3 as degeneracy-breaking perturbations. We conclude that Co(Al1-xCox)2O4 is below the theoretical critical point J2/J1=1/8, and that magnetic anisotropy assists in selecting a collinear long-range ordered ground state, which becomes more stable with increasing x due to a higher efficiency of O-Co3+-O as an interaction path compared to O-Al3+-O.

cond-mat.str-el↗

Optical phonons, spin correlations, and spin-phonon coupling in the frustrated pyrochlore magnets CdCr2O4 and ZnCr2O4

We report on infrared, Raman, magnetic susceptibility, and specific heat measurements on CdCr2O4 and ZnCr2O4 single crystals. We estimate the nearest-neighbor and next-nearest neighbor exchange constants from the magnetic susceptibility and extract the spin-spin correlation functions obtained from the magnetic susceptibility and the magnetic contribution to the specific heat. By comparing with the frequency shift of the infrared optical phonons above TN , we derive estimates for the spin-phonon coupling constants in these systems. The observation of phonon modes which are both Raman and infrared active suggest the loss of inversion symmetry below the Neel temperature in CdCr2O4 in agreement with theoretical predictions by Chern and coworkers [Phys. Rev. B 74, 060405 (2006)]. In ZnCr2O4 several new modes appear below TN, but no phonon modes could be detected which are both Raman and infrared active indicating the conservation of inversion symmetry in the low temperature phase.

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Magnetic susceptibility of the frustrated spinels ZnCr2O4, MgCr2O4 and CdCr2O4

We analyzed the magnetic susceptibilities of several Cr spinels using two recent models for the geometrically frustrated pyrochlore lattice, the Quantum Tetrahedral Mean Field model and a Generalized Constant Coupling model. Both models can describe the experimental data for ACr2 O4 (with A = Zn, Mg, and Cd) satisfactorily, with the former yielding a somewhat better agreement with experiment for A = Zn, Mg. The obtained exchange constants for nearest and next-nearest neighbors are discussed.

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Optical properties of ZnCr2Se4 - Spin-phonon coupling and electronic d-d-like excitations

We studied the optical properties of antiferromagnetic ZnCr2Se4 by infrared spectroscopy up to 28,000 cm-1 and for temperatures from 5 to 295 K. At the magnetic phase transition at 21 K, one of the four phonon modes reveals a clear splitting of 3 cm-1 as a result of spin-phonon coupling, the other three optical eigenmodes only show shifts of the eigenfrequencies. The antiferromagnetic ordering and the concomitant splitting of the phonon mode can be suppressed in a magnetic field of 7 T. At higher energies we observed a broad excitation band which is dominated by a two-peak-structure at about 18,000 cm-1 and 22,000 cm-1, respectively. These energies are in good agreement with the expected spin-allowed crystal-field transition of the Cr3+ ions. The unexpected strength of these forbidden onsite d-d transitions is attributed to a considerable hybridization of the selenium p with the chromium d orbitals.

cond-mat.str-el↗

Spin-driven Phase Transitions in ZnCr$_2$Se$_4$ and ZnCr$_2$S$_4$ Probed by High Resolution Synchrotron X-ray and Neutron Powder Diffraction

The crystal and magnetic structures of the spinel compounds ZnCr$_2$S$_4$ and ZnCr$_2$Se$_4$ were investigated by high resolution powder synchrotron and neutron diffraction. ZnCr$_2$Se$_4$ exhibits a first order phase transition at $T_N=21$ K into an incommensurate helical magnetic structure. Magnetic fluctuations above $T_N$ are coupled to the crystal lattice as manifested by negative thermal expansion. Both, the complex magnetic structure and the anomalous structural behavior can be related to magnetic frustration. Application of an external magnetic field shifts the ordering temperature and the regime of negative thermal expansion towards lower temperatures. Thereby, the spin ordering changes into a conical structure. ZnCr$_2$S$_4$ shows two magnetic transitions at $T_{N1}=15$ K and $T_{N2}=8$ K that are accompanied by structural phase transitions. The crystal structure transforms from the cubic spinel-type (space group $Fd$\={3}$m$) at high temperatures in the paramagnetic state, via a tetragonally distorted intermediate phase (space group $I4_1$ / $amd$) for $T_{N2} < T < T_{N1}$ into a low temperature orthorhombic phase (space group $I m m a$) for $T < T_{N2}$. The cooperative displacement of sulfur ions by exchange striction is the origin of these structural phase transitions. The low temperature structure of ZnCr$_2$S$_4$ is identical to the orthorhombic structure of magnetite below the Verwey transition. When applying a magnetic field of 5 T the system shows an induced negative thermal expansion in the intermediate magnetic phase as observed in ZnCr$_2$Se$_4$.

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Colossal magnetocapacitive effect in differently synthesized and doped CdCr2S4

In the present work, we address the question of an impurity-related origin of the colossal magnetocapacitive effect in the spinel system CdCr2S4. We demonstrate that a strong variation in the dielectric constant below the magnetic transition temperature or in external magnetic fields also arises in crystals prepared without chlorine. This excludes that an inhomogeneous distribution of chlorine impurities at the surface or in the bulk material gives rise to the unusual effects in the spinel multiferroics. In addition, we show that colossal magnetocapacitive effects can be also generated in chlorine-free ceramic samples of CdCr2S4, doped with indium.

cond-mat.mtrl-sci↗

Evidence for orthorhombic distortions in the ordered state of ZnCr$_2$O$_4$: A magnetic resonance study

We present an elaborate electron-spin resonance study of the low-energy dynamics and magnetization in the ordered phase of the magnetically frustrated spinel ZnCr$_2$O$_4$. We observe several resonance modes corresponding to different structural domains and found that the number of domains can be easily reduced by field-cooling the sample through the transition point. To describe the observed antiferromagnetic resonance spectra it is necessary to take into account an orthorhombic lattice distortion in addition to the earlier reported tetragonal distortion which both appear at the antiferromagnetic phase transition.

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Spin Frustration and Magnetic Exchange in Cobalt Aluminum Oxide Spinels

We report on x-ray diffraction, magnetic susceptibility, electron- spin resonance and heat- capacity studies of Co[Al_1-xCo_x]_2O_4 for Co concentrations 0 10 indicates the presence of strong spin frustration at least for x < 0.6. The frustration mechanism is attributed to competing nearest neighbor and next-nearest neighbor superexchange interactions between the A-site Co^2+ ions.

cond-mat.mtrl-sci↗

Polar phonons and spin-phonon coupling in HgCr2S4 and CdCr2S4

Polar phonons of HgCr2S4 and CdCr2S4 are studied by far-infrared spectroscopy as a function of temperature and external magnetic field. Eigenfrequencies, damping constants, effective plasma frequencies and Lyddane-Sachs-Teller relations, and effective charges are determined. Ferromagnetic CdCr2S4 and antiferromagnetic HgCr2S4 behave rather similar. Both compounds are dominated by ferromagnetic exchange and although HgCr2S4 is an antiferromagnet, no phonon splitting can be observed at the magnetic phase transition. Temperature and magnetic field dependence of the eigenfrequencies show no anomalies indicating displacive polar soft mode behavior. However, significant effects are detected in the temperature dependence of the plasma frequencies indicating changes in the nature of the bonds and significant charge transfer. In HgCr2S4 we provide experimental evidence that the magnetic field dependence of specific polar modes reveal shifts exactly correlated with the magnetization showing significant magneto-dielectric effects even at infrared frequencies.

cond-mat.str-el↗

Spin-phonon coupling in antiferromagnetic chromium spinels

The temperature dependence of eigenfrequencies and intensities of the IR active modes has been investigated for the antiferromagnetic chromium spinel compounds CdCr2O4, ZnCr2O4, ZnCr2S4, ZnCr2Se4, and HgCr2S4 by IR spectroscopy for temperatures from 5 K to 300 K. At the transition into the magnetically ordered phases, and driven by spin-phonon coupling, most compounds reveal significant splittings of the phonon modes. This is true for geometrically frustrated CdCr2O4, and ZnCr2O4, for bond frustrated ZnCr2S4 and for ZnCr2Se4, which also is bond frustrated, but dominated by ferromagnetic exchange. The pattern of splitting is different for the different compounds and crucially depends on the nature of frustration and of the resulting spin order. HgCr2S4, which is almost ferromagnetic, exhibits no splitting of the eigenfrequencies, but shows significant shifts due to ferromagnetic spin fluctuations.

cond-mat.str-el↗

Spin-phonon coupling in ZnCr2Se4

Spin-phonon coupling and magnetodielectric effects of ZnCr2Se4 were investigated by means of infrared (IR) spectroscopy as a function of temperature and magnetic field. ZnCr2Se4 is dominated by ferromagnetic exchange but undergoes antiferromagnetic order at T = 21 K. In the magnetically ordered phase the low-frequency IR active phonon splits, indicating strong dynamic anisotropy via magnetic exchange interactions. Antiferromagnetic order and concomitantly the phonon splitting is wiped out by external magnetic fields. Hence, ZnCr2Se4 is a prominent example of a spin-driven Jahn-Teller effect which can be fully suppressed in external magnetic fields.

cond-mat.str-el↗

Multiferroicity and colossal magneto-capacitance in Cr-thiospinels

The sulfur based Cr-spinels RCr2S4 with R = Cd and Hg exhibit the coexistence of ferromagnetic and ferroelectric properties together with a pronounced magnetocapacitive coupling. While in CdCr2S4 purely ferromagnetic order is established, in HgCr2S4 a bond-frustrated magnetic ground state is realized, which, however, easily can be driven towards a ferromagnetic configuration in weak magnetic fields. This paper shall review our recent investigation for both compounds. Besides the characterization of the magnetic properties, the complex dielectric permittivity was studied by means of broadband dielectric spectroscopy as well as measurements of polarization hysteresis and pyro-currents. The observed colossal magneto-capacitive effect at the magnetic transition seems to be driven by an enormous variation of the relaxation dynamics.

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Colossal magnetostriction and negative thermal expansion in the frustrated antiferromagnet ZnCr2Se4

A detailed investigation of ZnCr2Se4 is presented which is dominated by strong ferromagnetic exchange but orders antiferromagnetically at T_N = 21 K. Specific heat C and thermal expansion Delta L/L exhibit sharp first-order anomalies at the antiferromagnetic transition. T_N is strongly reduced and shifted to lower temperatures by external magnetic fields and finally is fully suppressed suggesting a field induced quantum critical behavior close to 60 kOe. Delta L/L(T) is unusually large and exhibits negative thermal expansion below 75 K down to T_N indicating strong frustration of the lattice. Magnetostriction Delta L/L(H) reveals colossal values (0.5x10^{-3}) comparable to giant magnetostriction materials. Electron-spin resonance, however, shows negligible spin-orbital coupling excluding orbitally induced Jahn-Teller distortions. The obtained results point to a spin-driven origin of the structural instability at T_N explained in terms of competing ferromagnetic and antiferromagnetic exchange interactions yielding strong bond frustration.

cond-mat.mtrl-sci↗

Spin-driven Phonon Splitting in Bond-frustrated ZnCr2S4

Utilizing magnetic susceptibility, specific heat, thermal expansion and IR spectroscopy we provide experimental evidence that the two subsequent antiferromagnetic transitions in ZnCr_2S_4 at T_N1 = 15 K and T_N2= 8 K are accompanied by significant thermal and phonon anomalies. The anomaly at T_N2 reveals a strong temperature hysteresis typical for a first-order transformation. Due to strong spin-phonon coupling both magnetic phase transitions induce a splitting of phonon modes, where at T_N1 the high-frequency and at T_N2 the low-frequency modes split. The anomalies and phonon splitting observed at T_N2 are strongly suppressed by magnetic field. Regarding the small positive Curie-Weiss temperature Theta= 8 K, we argue that this scenario of two different magnetic phases with concomitant different magneto-elastic couplings results from the strong competition of ferromagnetic and antiferromagnetic exchange of equal strength.

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Experimental evidence for competition of antiferromagnetic and ferromagnetic correlations in HgCr2S4

A detailed study of poly- and single crystalline samples of the normal spinel HgCr2S4 is reported. The structural refinement reveals enhanced values of the atomic displacements suggesting closeness to a structural instability. Magnetization, electron-spin resonance and specific-heat studies document strong ferromagnetic fluctuations close to 50 K and the occurrence of complex antiferromagnetic order at TN = 22 K. We found highly unconventional behavior resembling properties of a non-collinear antiferromagnet and soft ferromagnet dependent on temperature and magnetic field. Even weak external magnetic fields disturb the antiferromagnetic order and strongly enhance the ferromagnetic correlations. The conductivity shows an insulating character with non-monotonous temperature behavior and a metal-to-insulator like transition at 80 K well above the magnetic transition. The observed anomalies are related to bond frustration due to competing magnetic exchange interactions between the Cr ions.

cond-mat.mtrl-sci↗

Colossal magnetocapacitance and colossal magnetoresistance in HgCr2S4

We present a detailed study of the dielectric and charge transport properties of the antiferromagnetic cubic spinel HgCr2S4. Similar to the findings in ferromagnetic CdCr2S4, the dielectric constant of HgCr2S4 becomes strongly enhanced in the region below 60 - 80 K, which can be ascribed to polar relaxational dynamics triggered by the onset of ferromagnetic correlations. In addition, the observation of polarization hysteresis curves indicates the development of ferroelectric order below about 70 K. Moreover, our investigations in external magnetic fields up to 5 T reveal the simultaneous occurrence of magnetocapacitance and magnetoresistance of truly colossal magnitudes in this material.

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Multiferroic behavior in CdCr2X4 (X = S, Se)

The recently discovered multiferroic material CdCr2S4 shows a coexistence of ferromagnetism and relaxor ferroelectricity together with a colossal magnetocapacitive effect. The complex dielectric permittivity of this compound and of the structurally related CdCr2Se4 was studied by means of broadband dielectric spectroscopy using different electrode materials. The observed magnetocapacitive coupling at the magnetic transition is driven by enormous changes of the relaxation dynamics induced by the development of magnetic order.

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