arXiv subjects

M. A. Subramanian

Publications and source records attributed to M. A. Subramanian.

15 recordsLinked to original sources

arXiv2017

Spin order and dynamics in the diamond-lattice Heisenberg antiferromagnets CuRh2O4 and CoRh2O4

Antiferromagnetic insulators on the diamond lattice are candidate materials to host exotic magnetic phenomena ranging from spin-orbital entanglement to degenerate spiral ground-states and topological paramagnetism. Compared to other three-dimensional networks of magnetic ions, such as the geometrically frustrated pyrochlore lattice, the investigation of diamond-lattice magnetism in real materials is less mature. In this work, we characterize the magnetic properties of model A-site spinels CoRh2O4 (cobalt rhodite) and CuRh2O4 (copper rhodite) by means of thermo-magnetic and neutron scattering measurements and perform group theory analysis, Rietveld refinement, mean-field theory, and spin wave theory calculations to analyze the experimental results. Our investigation reveals that cubic CoRh2O4 is a canonical S=3/2 diamond-lattice Heisenberg antiferromagnet with a nearest neighbor exchange J = 0.63 meV and a Neel ordered ground-state below a temperature of 25 K. In tetragonally distorted CuRh2O4, competiting exchange interactions between up to third nearest-neighbor spins lead to the development of an incommensurate spin helix at 24 K with a magnetic propagation vector k = (0,0,0.79). Strong reduction of the ordered moment is observed for the S=1/2 spins in CuRh2O4 and captured by our 1/S corrections to the staggered magnetization. Our work identifies CoRh2O4 and CuRh2O4 as reference materials to guide future work searching for exotic quantum behavior in diamond-lattice antiferromagnets.

cond-mat.str-el↗

arXiv2013

First principles studies of SnTiO3 perovskite as a potential ferroelectric material

In the context of the search for environment-respectful, lead- and bismuth- free chemical compounds for devices such as actuators, SnTiO3 (ST) is investigated from first principles within DFT. Full geometry optimization provides a stable tetragonal structure relative to cubic one. From the equation of state the equilibrium volume of SnTiO3 is found smaller than ferroelectric PbTiO3 (PT) in agreement with a smaller Sn2+ radius. While ionic displacements exhibit similar trends between ST and PT a larger tetragonality (c/a ratio) for ST results in a larger polarization, PST = 1.1 C.m2. The analysis of the electronic band structure detailing the Sn-O and Ti-O interactions points to a differentiated chemical bonding and a reinforcement of the covalent bonding with respect to Pb homologue.

cond-mat.mtrl-sci↗

arXiv2009

Suppression of multiferroic order in hexagonal YMn1-xInxO3 ceramics

We have investigated the effects of substituting In for Mn on the antiferromagnetic phase transition in YMnO3 using magnetic, dielectric, and specific heat measurements. We prepared a set of isostructural phase pure hexagonal YMn$_{1-x}$In$_{x}$O$_{3}$ samples having x=0 to x=0.9, which exhibit a systematic decrease of the antiferromagnetic ordering temperature with increasing In content. The multiferroic phase, which develops below TN, appears to be completely suppressed for x$\geq$0.5 in the temperature range investigated, which can be attributed solely to the dilution of magnetic interactions as the crystal structure remains hexagonal. Similar to previous reports, we find an enhancement of the magnetocapacitive coupling on dilution with non-magnetic ions.

cond-mat.mtrl-sci↗

arXiv2009

Magnetically tunable dielectric materials

The coupling between localized spins and phonons can lead to shifts in the dielectric constant of insulating materials at magnetic ordering transitions. Studies on isostructural SeCuO3 (ferromagnetic) and TeCuO3 (antiferromagnetic) illustrate how the q-dependent spin-spin correlation function couples to phonon frequencies leading to a shift in the dielectric constant. A model is discussed for this spin-phonon coupling. The magnetodielectric coupling in multiferroic materials can be very large at a ferroelectric transition temperature. This coupling is investigated in the recently identified multiferroic Ni3V2O8.

cond-mat.mtrl-sci↗

arXiv2008

Effect of oxygen concentration on the structural and magnetic properties of LaRh1/2Mn1/2O3 thin films

Epitaxial LaRh1/2Mn1/2O3 thin films have been grown on (001)-oriented LaAlO3 and SrTiO3 substrates using pulsed laser deposition. The optimized thin film samples are semiconducting and ferromagnetic with a Curie temperature close to 100 K, a coercive field of 1200 Oe, and a saturation magnetization of 1.7muB per formula unit. The surface texture, structural, electrical, and magnetic properties of the LaRh1/2Mn1/2O3 films was examined as a function of the oxygen concentration during deposition. While an elevated oxygen concentration yields thin films with optimal magnetic properties, slightly lower oxygen concentrations result in films with improved texture and crystallinity.

cond-mat.mtrl-sci↗

arXiv2008

Dielectric and polarization experiments in high loss dielectrics: a word of caution

The recent quest for improved functional materials like high permittivity dielectrics and/or multiferroics has triggered an intense wave of research. Many materials have been checked for their dielectric permittivity or their polarization state. In this report, we call for caution when samples are simultaneously displaying insulating behavior and defect-related conductivity. Many oxides containing mixed valent cations or oxygen vacancies fall in this category. In such cases, most of standard experiments may result in effective high dielectric permittivity which cannot be related to ferroelectric polarization. Here we list few examples of possible discrepancies between measured parameters and their expected microscopic origin.

cond-mat.mtrl-sci↗

arXiv2005

First principles investigation of the electronic structure of La2MnNiO6: A room-temperature insulating ferromagnet

Using first principles calculations within DFT based on the full potential APW+lo method, we calculated the electronic and magnetic structures for the ferromagnetic and antiferromagnetic states of La2MnNiO6 and analyzed the site projected density of states and electronic band structures. Our calculations show that the ground state of La2MnNiO6 is ferromagnetic insulating with the magnetization in agreement with Hund's first rule and experimental findings.

cond-mat.str-el↗

arXiv2004

Evidence for power-law frequency dependence of intrinsic dielectric response in the CaCu$_{3}$Ti$_{4}$O$_{12}$

We investigated the dielectric response of CaCu$_3$Ti$_4$O$_{12}$ (CCTO) thin films grown epitaxially on LaAlO$_3$ (001) substrates by Pulsed Laser Deposition (PLD). The dielectric response of the films was found to be strongly dominated by a power-law in frequency, typical of materials with localized hopping charge carriers, in contrast to the Debye-like response of the bulk material. The film conductivity decreases with annealing in oxygen, and it suggests that oxygen deficit is a cause of the relatively high film conductivity. With increase of the oxygen content, the room temperature frequency response of the CCTO thin films changes from the response indicating the presence of some relatively low conducting capacitive layers to purely power law, and then towards frequency independent response with a relative dielectric constant $ε'\sim10^2$. The film conductance and dielectric response decrease upon decrease of the temperature with dielectric response being dominated by the power law frequency dependence. Below $\sim$80 K, the dielectric response of the films is frequency independent with $ε'$ close to $10^2$. The results provide another piece of evidence for an extrinsic, Maxwell-Wagner type, origin of the colossal dielectric response of the bulk CCTO material, connected with electrical inhomogeneity of the bulk material.

cond-mat.mtrl-sci↗

arXiv2004

An experimental and computational investigation of structure and magnetism in pyrite Co$_{1-x}$Fe$_x$S$_2$: Chemical bonding and half-metallicity

Bulk samples of the pyrite chalcogenide solid solutions Co$_{1-x}$Fe$_x$S$_2$ 0 <= x <= 0.5, have been prepared and their crystal structures and magnetic properties studied by X-ray diffraction and SQUID magnetization measurements. Across the solution series, the distance between sulfur atoms in the persulfide (S$_2^{2-}$) unit remains nearly constant. First principles electronic structure calculations using experimental crystal structures as inputs point to the importance of this constant S-S distance, in helping antibonding S-S levels pin the Fermi energy. In contrast hypothetical rock-salt CoS is not a good half metal, despite being nearly isostructural and isoelectronic. We use our understanding of the Co$_{1-x}$Fe$_x$S$_2$ system to make some prescriptions for new ferromagnetic half-metals.

cond-mat.mtrl-sci↗

arXiv2004

Valence-electron transfer and a metal-insulator transition in a strongly correlated perovskite oxide

We present transport and thermal data for the quadruple-perovskites MCu3(Ti1-xRux)4O12 where 0 < x < 1. A metal-insulator transition (MIT) occurs for Ru concentrations x~0.75. At the same time, the Cu2+ antiferromagnetic state is destroyed and it's magnetic entropy suppressed by Ru on a 1:1 basis. This implies that each Ru transfers an electron to a Cu ion and thus the MIT correlates with filling the Cu 3d shell. The Cu spin entropy in this strongly correlated electron material provides a unique probe among MIT systems.

cond-mat.mtrl-sci↗

arXiv2003

Magnetodielectric Effects from Spin Fluctuations in Isostructural Ferromagnetic and Antiferromagnetic Systems

We report on the effects of spin fluctuations, magnetic ordering, and external magnetic field on the dielectric constant of the ferromagnet SeCuO3, and the antiferromagnet TeCuO3. A model based on the coupling between uniform polarization and the q-dependent spin-spin correlation function is presented to explain the different behaviors for these isostructural compounds. The large magnetocapacitance near the transition temperature in the ferromagnet SeCuO3 suggests routes to enhancing the magnetodielectric response for practical applications.

cond-mat.mtrl-sci↗

arXiv2002

Colossal Dielectric Constants in Braced Lattices with Defects

The dielectric constant of CaCu3Ti4O12 is measured with a different electrode geometry than previous measurements. Similar colossal values are obtained showing that they are "intrinsic" to the material. We show that in braced structures such as CaCu3Ti4O12, a small concentration O(10-3) of defects, which disrupt the bracing and relax between different equivalent configurations, can lead to colossal dielectric constants above a characteristic temperature. The dielectric constant e(w,T) has a frequency and temperature dependence of the same form as found experimentally.

cond-mat↗

arXiv2002

Charge transfer in the high dielectric constant materials CaCu3Ti4O12 and CdCu3Ti4O12

The cubic perovskite-related ceramic CaCu3Ti4O12 has a very high static dielectric constant ~10000 at room temperature (RT), which drops to about 100 below about 100 K. Substituting Cd for Ca reduces the RT value of the dielectric constant by over an order of magnitude. The large the dielectric constant may be due to an internal barrier layer capacitance (IBLC) effect. Infrared optical properties show a low-frequency mode that increases dramatically in strength at low temperature, suggesting a change in the effective charges and a breakdown of the IBLC model due to a semiconductor-to-insulator transition.

cond-mat.str-el↗

arXiv2000

Local lattice disorder in the geometrically-frustrated spin glass pyrochlore Y2Mo2O7

The geometrically-frustrated spin glass Y2Mo2O7 has been considered widely to be crystallographically ordered with a unique nearest neighbor magnetic exchange interaction, J. To test this assertion, we present x-ray-absorption fine-structure results for the Mo and Y K edges as a function of temperature and compare them to results from a well-ordered pyrochlore, Tl2Mn2O7. We find that the Mo-Mo pair distances are significantly disordered at approximately right angles to the Y-Mo pairs. These results strongly suggest that lattice disorder nucleates the spin-glass phase in this material.

cond-mat.stat-mech↗

arXiv1998

Spin Dynamics of the Magnetoresistive Pyrochlore Tl_2Mn_2O_7

Neutron scattering has been used to study the magnetic order and spin dynamics of the colossal magnetoresistive pyrochlore Tl_2Mn_2O_7. On cooling from the paramagnetic state, magnetic correlations develop and appear to diverge at T_C (123 K). In the ferromagnetic phase well defined spin waves are observed, with a gapless ($Δ<0.04$ meV) dispersion relation E=Dq^{2} as expected for an ideal isotropic ferromagnet. As T approaches T_C from low T, the spin waves renormalize, but no significant central diffusive component to the fluctuation spectrum is observed in stark contrast to the La$_{1-x}$(Ca,Ba,Sr)$_x$MnO$_3$ system. These results argue strongly that the mechanism responsible for the magnetoresistive effect has a different origin in these two classes of materials.

cond-mat.str-el↗