arXiv subjects

S. M. Yusuf

Publications and source records attributed to S. M. Yusuf.

At least 37 records · Page 2Linked to original sources

arXiv2022

Observation of anisotropic thermal expansion and Jahn-Teller effect in double perovskites Sr$_{2-x}$La$_x$CoNbO$_6$ using neutron diffraction

We use temperature dependent neutron powder diffraction (NPD) to investigate the structural changes and magnetic interactions in double perovskite Sr$_{2-x}$La$_x$CoNbO$_6$ ($x=$ 0.4 and 0.6). A structural phase transition from tetragonal ($I4/m$) to monoclinic ($P2_1/n$) is observed between $x=$ 0.4 and 0.6 samples. Interestingly, temperature evolution of the unit cell parameters follow the Grüneisen approximation, and the analysis suggest the isotropic thermal expansion in case of the $x=$ 0.4 sample, whereas the $x=$ 0.6 sample shows the anisotropy where the thermal expansion along the $c$-axis significantly deviates from the Grüneisen function. We observe the $z$-out Jahn-Teller distortion in the CoO$_6$ and consequently $z$-in distortion in the adjacent NbO$_6$ octahedra. With increase in the La substitution, a decrease in the degree of octahedral distortion is evident from the significant reduction in the local distortion parameter $Δ$ around the B-site atoms.

cond-mat.str-el↗

arXiv2022

Magnetism of the 2D honeycomb layered Na2Ni2TeO6 compound driven by intermediate Na-layer crystal-structure

The microscopic spin-spin correlations in the 2D layered spin-1 honeycomb lattice compound Na2Ni2TeO6 have been investigated by neutron diffraction and inelastic neutron scattering. The honeycomb lattice of spin-1 Ni2+ ions, within the crystallographic ab planes, are well separated along the c axis by an intermediate Na layer whose crystal structure contains chiral nuclear density distributions of Na ions. The chirality of the alternating Na layers is opposite. Such alternating chirality of the Na layer dictates the magnetic periodicity along the c axis where an up-up-down-down spin arrangement of the in-plane zigzag AFM structure is found. Besides, the above described commensurate (CM) zigzag AFM order state is found to coexist with an incommensurate (ICM) AFM state below the TN ~ 27.5 K. The ICM state is found to appear at much higher temperature ~ 50 K and persists down to lowest measured temperature of 1.7 K. Our reverse Monte Carlo (RMC) analysis divulges a two dimensional (2D) magnetic correlations (within the ab plane) of the ICM AFM state over the entire temperature range 1.7-50 K. Further, the spin-Hamiltonian has been determined by carrying out inelastic neutron scattering experiments and subsequent linear spin-wave theory analysis which reveals the presence of competing inplane exchange interactions up to 3 rd nearest neighbours consistent with the zigzag AFM ground state, and weak interplanar interaction as well as a weak single-ion-anisotropy. The values of the exchange constants yield that Na2Ni2TeO6 is situated well inside the zigzag AFM phase (spans over a wide ranges of J2/J1 and J3/J1 values) in the theoretical phase diagram. The present study, thus, provides a detailed microscopic understanding of the magnetic correlations and divulges the intertwining magneto-structural correlations.

cond-mat.str-el↗

arXiv2022

Collinear antiferromagnetic order in spin-$\frac52$ triangle lattice antiferromagnet Na$_3$Fe(PO$_4$)$_2$

We set forth the structural and magnetic properties of the frustrated spin-$5/2$ triangle lattice antiferromagnet Na$_3$Fe(PO$_4$)$_2$ examined via x-ray diffraction, magnetization, heat capacity, and neutron diffraction measurements on the polycrystalline sample. No structural distortion was detected from the temperature-dependant x-ray diffraction down to 12.5 K, except a systematic lattice contraction. The magnetic susceptibility at high temperatures agrees well with the high-temperature series expansion for a spin-$5/2$ isotropic triangular lattice antiferromagnet with an average exchange coupling of $J/k_{\rm B} \simeq 1.8$ K rather than a one-dimensional spin-$5/2$ chain model. This value of the exchange coupling is consistently reproduced by the saturation field of the pulse field magnetization data. It undergoes a magnetic long-range-order at $T_{\rm N} \simeq 10.4$ K. Neutron diffraction experiments elucidate a collinear antiferromagnetic ordering below $T_{\rm N}$ with the propagation vector $k = (1,0,0)$. An intermediate value of frustration ratio ($f \simeq 3.6$) reflects moderate frustration in the compound which is corroborated by a reduced ordered magnetic moment of $\sim 1.52$ $μ_{\rm B}$ at 1.6 K, compared to its classical value ($5 μ_{\rm B}$). Magnetic isotherms exhibit a change of slope envisaging a field induced spin-flop transition at $H_{\rm SF}\simeq3.2$ T. The magnetic field vs temperature phase diagram clearly unfold three distinct phase regimes, reminiscent of a frustrated magnet with in-plane (XY-type) anisotropy.

cond-mat.mtrl-sci↗

arXiv2021

Unraveling diffusion kinetics of honeycomb structured Na$_2$Ni$_2$TeO$_6$ as a high-potential and stable electrode for sodium-ion batteries

In search of the potential cathode materials for sodium-ion batteries and to understand the diffusion kinetics, we report the detailed analysis of electrochemical investigation of honeycomb structured Na$_{2}$Ni$_{2}$TeO$_{6}$ material using cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), galvanostatic charge-discharge (GCD) and galvanostatic intermittent titration technique (GITT). We found the discharge capacities of 82 and 77 mAhg$^{-1}$ at 0.05~C and 0.1~C current rates, respectively, and the mid-working potential of $\approx$3.9~V at 1~C and high capacity retention of 80\% after 500 cycles at 0.5~C as well as excellent rate capability. The analysis of CV data at different scan rates reveals the pseudo-capacitive mechanism of sodium-ion storage. Interestingly, the {\it in-situ} EIS measurements show a systematic change in the charge-transfer resistance at different charge/discharge stages as well as after different number of cycles. The diffusion coefficient extracted using CV, EIS and GITT lies mainly in the range of 10$^{-10}$ to 10$^{-12}$ cm$^{2}$s$^{-1}$ and the de-insertion/insertion of Na$^+$-ion concentration during electrochemical cycling is consistent with the ratio of Ni$^{3+}$/Ni$^{2+}$ valence state determined by photoemission study. Moreover, the post-cyclic results of retrieved active material show very stable structure and morphology even after various charge-discharge cycles. Our detailed electrochemical investigation and diffusion kinetics studies establish the material as a high working potential and long life electrode for sodium-ion batteries.

physics.chem-ph↗

arXiv2021

Magnetic properties of S = 5/2 anisotropic triangular chain Bi3FeMo2O12

Competing magnetic interactions in low-dimensional quantum magnets can lead to the exotic ground state with fractionalized excitations. Herein, we present our results on an S = 5/2 quasi-one-dimensional spin system Bi3FeMo2O12. The structure of Bi3FeMo2O12 consists of very well separated, infinite zig-zag S = 5/2 spin chains. The observation of a broad maximum around 10 K in the magnetic susceptibility suggests the presence of short-range spin correlations. Magnetic susceptibility data do not fit to S=5/2 uniform spin chain model due to the presence of 2nd nearest-neighbor coupling (J2) along with the 1st nearest-neighbor coupling J1 of the zig-zag chain. The electronic structure calculations infer that the value of J1 is comparable with J2 (J2/J1~1.1) with a negligible inter-chain interaction (J'/J ~ 0.01), implying that Bi3FeMo2O12 is a highly frustrated triangular chain system. The absence of magnetic long-range ordering down to 0.2 K is seen in the heat capacity data, despite a relatively large antiferromagnetic Curie-Weiss temperature of -40 K. The magnetic heat capacity follows nearly a linear behavior at low temperatures indicating that the S = 5/2 anisotropic triangular chain exhibits the gapless excitations.

cond-mat.str-el↗

arXiv2021

Mechanism of Na-ionic conduction in the high efficient layered battery material Na2Mn3O7

The ionic conduction properties of the technologically important two-dimensional (2D) layered battery material Na2Mn3O7, with exceptional small-voltage hysteresis between charge and discharge curves, have been investigated as a function of temperature and frequency by an impedance spectroscopy. The detailed analyses of the impedance data in the form of dc-conductivity, ac-conductivity, electrical modulus, dielectric constant and complex polarizability reveal a long-range Na-ionic conductivity with negligible contribution from a local dipole relaxation. A significant enhancement (~10^4 times) of the Na-ion conductivity has been found with the increasing temperature from 353 K to 713 K. The temperature dependent conductivity reveals thermally activated conduction process with activation energies of 0.161 and 0.377 eV over the two temperature regions of 383-518 K and 518-713 K, respectively. AC conductivity study reveals a long-range hopping process for the conduction of charge carriers with a sharp increase of the hopping range at 518 K. The scaling study of the ac-conductivity reveals that the frequency-activated conductivity (above 10^4 Hz at 353 K) is mainly controlled by the critical frequency that increases with the increasing temperature. The Na-ion conduction in Na2Mn3O7 occurs predominantly by a correlated barrier hopping process. Besides, a correlation between ionic conduction and crystal structure has been established by x-ray and neutron diffraction study. We have further shown that the conductivity of Na2Mn3O7 can be enhanced by reduction of the stacking faults in the crystal structure. Our study facilitates the understanding of the microscopic ionic conduction mechanism in the highly efficient 2D battery material Na2Mn3O7 having high energy storage capacity and high structural stability, paving way for the discovery of materials for battery applications.

cond-mat.mtrl-sci↗

arXiv2020

Structure, magnetism and electronic properties in 3$d$-5$d$ based double perovskite (Sr$_{1-x}$Ca$_x$)$_2$FeIrO$_6$ (0 $\leq$ $x$ $\leq$ 1): A combined experimental and theoretical investigation

The 3$d$-5$d$ based double perovskites offer an ideal playground to study the interplay between electron correlation ($U$) and spin-orbit coupling (SOC) effect, showing exotic physics. The Sr$_2$FeIrO$_6$ is an interesting member in this family with ionic distribution of Fe$^{3+}$ (3$d^5$) and Ir$^{5+}$ (5$d^4$) where the later is believed to be nonmagnetic under the picture of strong SOC. Here, we report detailed investigation of structural, magnetic and electronic transport properties along with electronic structure calculations in (Sr$_{1-x}$Ca$_x$)$_2$FeIrO$_6$ series with $x$ from 0 to 1. While the basic interactions such as, $U$ and SOC are unlikely to be modified but a structural modification is expected due to ionic size difference between Sr$^{2+}$ and Ca$^{2+}$ which would influence other properties such as crystal field effect and band widths. While a nonmonotonic changes in lattice parameters are observed across the series, the spectroscopic investigations reveal that 3+/5+ charge state of Fe/Ir continue till end of the series. An analysis of magnetic data suggests similar nonmonotonic evolution of magnetic parameters with doping. Temperature dependent crystal structure as well as low temperature (5 K) magnetic structure have been determined from neutron powder diffraction measurements. The whole series shows insulating behavior. The electronic structure calculations show, SOC enhanced, a noncollinear antiferromagnetic and Mott-type insulating state is the stable ground state for present series with a substantial amount of orbital moment, but less than the spin magnetic moment, at the Ir site and the magnetocrystalline anisotropy. The obtained results imply that the Ca$^{2+}$ has large influence on the magnetic and transport properties, further showing a large agreement between experimental results as well as theoretical calculations.

cond-mat.str-el↗

arXiv2020

Unconventional superparamagnetic behavior in the modified cubic spinel compound LiNi$_{0.5}$Mn$_{1.5}$O$_{4}$

Structural, electronic, and magnetic properties of modified cubic spinel compound LiNi$_{0.5}$Mn$_{1.5}$O$_{4}$ are studied via x-ray diffraction, resistivity, DC and AC magnetization, heat capacity, neutron diffraction, $^7$Li nuclear magnetic resonance, magnetocaloric effect, magnetic relaxation, and magnetic memory effect experiments. We stabilized this compound in a cubic structure with space group $P4_{3}32$. It exhibits semiconducting character with an electronic band gap of $Δ/k_{\rm B} \simeq 0.4$ eV. The interaction within each Mn$^{4+}$ and Ni$^{2+}$ sub-lattice and between Mn$^{4+}$ and Ni$^{2+}$ sublattices is found to be ferromagnetic (FM) and antiferromagnetic (AFM), respectively which leads to the onset of a ferrimagnetic transition at $T_{\rm C} \simeq 125$~K. The reduced values of frustration parameter ($f$) and ordered moments reflect magnetic frustration due to competing FM and AFM interactions. From the $^7$Li NMR shift vs susceptibility plot, the average hyperfine coupling between $^7$Li nuclei and Ni$^{2+}$ and Mn$^{4+}$ spins is calculated to be $\sim 672.4$~Oe/$μ_{\rm B}$. A detailed critical behaviour study is done in the vicinity of $T_{\rm C}$ using modified-Arrott plot, Kouvel-Fisher plot, and universal scaling of magnetization isotherms. The estimated critical exponents correspond to the 3D XY universality class. A large magneto-caloric effect is observed with a maximum isothermal change in entropy $ΔS_m \simeq - 11.3$~J/Kg-K and a maximum relative cooling power $RCP \simeq 604$~J/Kg for 9~T magnetic field change. The imaginary part of the AC susceptibility depicts a strong frequency dependent hump at $T=T_{\rm f2}$ well below the blocking temperature $T_{\rm b}\simeq120$~K. The Arrhenius behaviour of frequency dependent $T_{\rm f2}$ and the absence of ZFC memory confirm the existence of superparamagnetism in the ferrimagnetically ordered state.

cond-mat.mtrl-sci↗

arXiv2020

Temperature Dependent Na-ion Conduction and its Pathways in the Crystal Structure of the Layered Battery Material Na$_2$Ni$_2$TeO$_6$

Na-ion conduction, and correlations between Na-ion conduction pathways and crystal structure have been investigated as a function of temperature in the layered battery material Na2Ni2TeO6 by impedance spectroscopy and neutron diffraction, respectively. The impedance data reveal an ionic conductivity 2x10-4 S/m at 323 K which strongly enhances with increasing temperature and attains a high value of ~ 0.03 S/m at 423 K. The temperature dependent conductivity data show an Arrhenius type behavior with average activation energy (Ea) of ~ 0.58(3) eV for T > 383 K. By employing soft-bond valence sum analysis of the neutron diffraction patterns we experimentally demonstrate the site-specific Na-ion conductions, through visualization of microscopic sodium-ion conduction pathways, and verify the recent theoretical results of Molecular dynamic simulation. Our results reveal two-dimensional Na-ion conduction pathways that are confined within the ab planes of Na layers. Crystal structural study indicates that the layered structure involving Na ion layers is responsible for high ionic conductivity, and the local crystallographic environment of Na ion sites is responsible for site-specific conductivity. Our study further reveals that up to 500 K, the ionic conduction is governed by the Na ions located at the Na1 and Na2 sites, whereas, all the Na ions located at the three Na-sites contribute to the conduction process above 500 K. Our neutron diffraction study also establishes that the crystal structure of Na2Ni2TeO6 is stable at least up to 725 K (the highest measured temperature), however, with an anisotropic thermal expansion (c/a ~ 3).

cond-mat.mtrl-sci↗

arXiv2020

Excitations in the spin-1 trimer chain compound CaNi3P4O14: gapped dispersive spinwaves to gapless magnetic excitations

Magnetic excitations and the spin Hamiltonian of the spin-1 J1-J1-J2 trimer chain compound CaNi3P4O14 have been investigated by inelastic neutron scattering. Experimental data reveal gapped dispersive spin wave excitations in the 3D long-range ordered magnetic state (TC = 16 K), and gapless magnetic excitations above the TC. Simulated magnetic excitations, by using the linear spin wave theory, for a model of coupled trimer spin-chains provide a good description of the observed experimental data. The analysis reveals both ferromagnetic J1 and J2 interactions within the chains, and an antiferromagnetic interchain interaction J3 between chains. The strengths of the J1 and J2 are found to be closer (J2/J1 ~ 0.81), and J3 is determined to be weaker (J3/ J1 ~ 0.69), which is consistent with the spin chain type crystal structure. Presence of a weak single-ion-anisotropy (D/J=0.19) is also revealed. The strengths and signs of exchange interactions explain why the 1/3 magnetization is absent in the studied spin-1 compound CaNi3P4O14 in contrast to its S= 5/2 counterpart Mn based isostructural compound. The signs of the exchange interactions are in agreement with that obtained from the reported DFT calculations, whereas, their strengths are found to be significantly different. The relatively strong value of the J3 in CaNi3P4O14 gives a conventional 3D type magnetic ordering below the TC, however, retains its 1D character above the TC. The present experimental study also reveals a sharp change of single-ion anisotropy across the TC indicating that the stability of the 3D magnetic ordering in CaNi3P4O14 is ascribed to the local magnetic anisotropy in addition to interchain interactions. The present study divulges the importance of full knowledge of the exchange interactions in trimer spin chain compounds to understand their exotic magnetic properties, such as 1/3 magnetization plateau.

cond-mat.str-el↗

arXiv2020

Probing low temperature non-equilibrium magnetic state in Co$_{2.75}$Fe$_{0.25}$O$_{4+δ}$ spinel oxide using dc magnetization, ac susceptibility and neutron diffraction experiments

The low temperature lattice structure and magnetic properties of Co$_{2.75}$Fe$_{0.25}$O$_4$ ferrite have been investigated using experimental results from synchrotron x-ray diffraction (SXRD), dc magnetization, ac susceptibility, neutron diffraction and neutron depolarization techniques. The samples have been prepared by chemical co-precipitation of the Fe and Co nitrates solution in high alkaline medium and subsequent thermal annealing of the precipitates in the temperature range of 200- 900 $^\circ$C. Rietveld refinement of the SXRD patterns at room temperature indicated two-phased cubic spinel structure for the samples annealed at temperatures 200-600 $^\circ$C. The samples annealed at temperatures 700 $^\circ$C and 900 $^\circ$C (CF90) have been best fitted with single phased lattice structure. Refinement of the neutron diffraction patterns in the temperature range of 5-300 K confirmed antiferromagnetic (AFM) Co$_3$O$_4$ and ferrimagnetic (FIM) Co$_{2.75}$Fe$_{0.25}$O$_4$ phases for the sample annealed at 600 $^\circ$C and single FIM phase of Co$_{2.75}$Fe$_{0.25}$O$_4$ for the CF90 sample. Magnetic measurements have shown a non-equilibrium magnetic structure, consisting of the high temperature FIM phase and low temperature AFM phase. The magnetic phases are sensitive to magnetic fields, where high temperature phase is suppressed at higher magnetic fields by enhancing the low temperature AFM phase, irrespective of annealing temperature of the samples.

cond-mat.str-el↗

arXiv2019

Spin dynamics and unconventional magnetism in insulating La$_{(1-2x)}$Sr$_{2x}$Co$_{(1-x)}$Nb$_{x}$O$_3$

We study the structural, magnetic, transport and electronic properties of LaCoO$_3$ with Sr/Nb co-substitution, i.e., La$_{(1-2x)}$Sr$_{2x}$Co$_{(1-x)}$Nb$_{x}$O$_3$ using x-ray and neutron diffraction, dc and ac-magnetization, neutron depolarization, dc-resistivity and photoemission measurements. The powder x-ray and neutron diffraction data were fitted well with the rhombohedral crystal symmetry (space group \textit{R$\bar{3}$c}) in Rietveld refinement analysis. The calculated effective magnetic moment ($\approx$3.85~$μ_B$) and average spin ($\approx$1.5) of Co ions from the analysis of magnetic susceptibility data are consistent with 3+ state of Co ions in intermediate-spin (IS) and high-spin (HS) states in the ratio of $\approx$50:50, i.e., spin-state of Co$^{3+}$ is preserved at least up to $x=$ 0.1 sample. Interestingly, the magnetization values were significantly increased with respect to the $x=$ 0 sample, and the M-H curves show non-saturated behavior up to an applied maximum magnetic field of $\pm$70 kOe. The ac-susceptibility data show a shift in the freezing temperature with excitation frequency and the detailed analysis confirm the slower dynamics and a non-zero value of the Vogel-Fulcher temperature T$_0$, which suggests for the cluster spin glass. The unusual magnetic behavior indicates the presence of complex magnetic interactions at low temperatures. The dc-resistivity measurements show the insulating nature in all the samples. However, relatively large density of states $\approx$10$^{22}$ eV$^{-1}$cm$^{-3}$ and low activation energy $\approx$130~meV are found in $x=$ 0.05 sample. Using x-ray photoemission spectroscopy, we study the core-level spectra of La 3$d$, Co 2$p$, Sr 3$d$, and Nb 3$d$ to confirm the valence state.

cond-mat.str-el↗

arXiv2018

Zigzag spin chains in the spin-5/2 antiferromagnet Ba$_2$Mn(PO$_4)_2$

Magnetic properties and magnetic structure of the Ba$_{2}$Mn(PO$_{4}$)$_{2}$ antiferromagnet featuring frustrated zigzag chains of $S=\frac{5}{2}$ Mn$^{2+}$ ions are reported based on neutron diffraction, density-functional band-structure calculations, as well as temperature- and field-dependent measurements of the magnetization and specific heat. A magnetic transition at $T_N\simeq 5$\,K marks the onset of the antiferromagnetic order with the propagation vector ${\mathbf k} = (\frac12\, 0\, \frac12)$ and ordered moment of $4.33\pm0.08~μ_B$/Mn$^{2+}$ at 1.5\,K, pointing along the $c$ direction. Direction of the magnetic moment is chosen by the single-ion anisotropy, which is relatively weak compared to the isostructural Ni$^{2+}$ compound. Geometrical frustration has strong impact on thermodynamic properties of Ba$_2$Mn(PO$_4)_2$, but manifestations of the frustration are different from those in Ba$_2$Ni(PO$_4)_2$, where frustration by isotropic exchange couplings is minor, yet strong and competing single-ion anisotropies are present. A spin-flop transition is observed around 2.5\,T. The evaluation of the magnetic structure from the ground state via the spin-flop state to the field-polarized ferromagnetic state has been revealed by a comprehensive neutron diffraction study as a function of magnetic field below $T_N$. Finally, a magnetic phase diagram in the $H-T$ plane is obtained.

cond-mat.str-el↗

arXiv2018

Structural, Electrical, and Magnetic Properties of La2Ni1.5Mn0.5O6 double perovskites

Among multifunctional double perovskite oxides, La2NiMnO6 has recently drawn significant attention due to its importance both in terms of understanding of fundamental physics and potential for device applications. The relative alteration in Ni:Mn ratio strongly influences the structural, magnetic and electrical properties of La2NiMnO6. In the present study, La2Ni1.5Mn0.5O6 sample with Ni:Mn = 3:1 ratio has been prepared using sol-gel method and modifications of the above physical properties from that of a stiochiometric sample of La2NiMnO6 are discussed. Rietveld analysis of X-ray diffraction data shows that La2Ni1.5Mn0.5O6 samples belong to a major monoclinic structural phase (P21/n), with partially disordered arrangement of Ni and Mn ions. Magnetic characterization and X-ray absorption near edge structure analysis reveal ferromagnetic ordering around 260 K between Ni2+ and Mn4+ ions while spin glass like behavior is revealed at ~45 K. Semiconducting nature of the sample was confirmed from temperature dependent resistivity measurements as well as from the I-V characteristics measured at room temperature.

cond-mat.mtrl-sci↗

arXiv2016

Spin reorientation in NdFe$_{0.5}$Mn$_{0.5}$O$_{3}$: Neutron scattering and \emph{Ab-initio} study

The structural, magnetic, and electronic properties of NdFe$_{0.5}$Mn$_{0.5}$O$_3$ have been studied in detail using bulk magnetization, neutron/x-ray diffraction and first principles density functional theory calculations. The material crystallizes in the orthorhombic $Pbnm$ structure, where both Mn and Fe occupy the same crystallographic site ($4b$). Mn/Fe sublattice of the compound orders in to a G-type antiferromagnetic phase close to 250\,K where the magnetic structure belongs to $Γ_{1}$ irreducible representation with spins aligned along the crystallographic $b$ direction. This is unconventional in the sense that most of the orthoferrites and orthochromites order in the $Γ_{4}$ representation below the Néel temperature.This magnetic structure then undergoes a complete spin reorientation transition with temperature in the range 75\,K$\gtrsim$ T $\gtrsim$ 25\,K where the magnetic structure exists as a sum of two irreducible representations ($Γ_{1}$+$Γ_{2}$) as seen from neutron diffraction measurements. At 6\,K, the magnetic structure belongs entirely to $Γ_{2}$ representation with spins aligned antiferromagnetically along the crystallographic $c$ direction having a small ferromagnetic component ($F_x$). The unusual spin reorientation and correlation between magnetic ground state and electronic structure have been investigated using first principles calculations within GGA+U and GGA+U+SO formalisms.

cond-mat.str-el↗

arXiv2016

Non-collinear antiferromagnetism of coupled spins and pseudospins in the double perovskite La2CuIrO6

We report the structural, magnetic and thermodynamic properties of the double perovskite compound La2CuIrO6 from X-ray, neutron diffraction, neutron depolarization, dc magnetization, ac susceptibility, specific heat, muon-spin-relaxation (uSR), electron-spin-resonance (ESR) and nuclear magnetic resonance (NMR) measurements. Below ~113 K, short-range spin-spin correlations occur within the Cu2+ sublattice. With decreasing temperature, the Ir4+ sublattice progressively involves in the correlation process. Below T = 74 K, the magnetic sublattices of Cu (spin s = 1/2) and Ir (pseudospin j = 1/2) in La2CuIrO6 are strongly coupled and exhibit an antiferromagnetic phase transition into a non-collinear magnetic structure accompanied by a small uncompensated transverse moment. A weak anomaly in ac-susceptibility as well as in the NMR and μSR spin lattice relaxation rates at 54 K is interpreted as a cooperative ordering of the transverse moments which is influenced by the strong spin-orbit coupled 5d ion Ir4+. We argue that the rich magnetic behaviour observed in La2CuIrO6 is related to complex magnetic interactions between the strongly correlated spin-only 3d ions with the strongly spin-orbit coupled 5d transition ions where a combination of the spin-orbit coupling and the low-symmetry of the crystal lattice plays a special role for the spin structure in the magnetically ordered state.

cond-mat.str-el↗

arXiv2016

Zigzag antiferromagnetic ground state with anisotropic correlation lengths in the quasi-2D honeycomb lattice compound Na2Co2TeO6

The crystal structure, magnetic ground state, and the temperature dependent microscopic spin-spin correlations of the frustrated honeycomb lattice antiferromagnet Na2Co2TeO6 have been investigated by powder neutron diffraction. A three dimensional (3D) long-range antiferromagnetic ordering has been found below TN ~ 24.8 K. The magnetic ground state, determined to be zigzag antiferromagnet [k = (1/2 0 0)], occurs due to the competing exchange interactions up to third nearest neighbors within the honeycomb lattice. The exceptional existence of a limited magnetic correlation length along the c axis (perpendicular to the honeycomb layers in the ab planes) has been found within the 3D long-range ordered state, even at 1.8 K, well below TN. The observed limited correlation along the c axis is explained by the disorder distribution of the Na ions within the intermediate layers. The reduced ordered moments mCo(1) = 2.77(3) muB/Co2+ and mCo(2) = 2.45(2) muB/Co2+ at 1.8 K reflect the persistence of spin fluctuations in the ordered state. Above TN, the presence of short-range magnetic correlations, manifested by broad diffuse magnetic peaks, has been found. Reverse Monte Carlo analysis of the experimental diffuse magnetic scattering data reveals that the spin correlations are mainly confined within the 2D honeycomb layers (ab plane) with a correlation length of ~ 12 Å at 25 K. The nature of spin arrangements is found to be similar in both the short-range and long-range ordered magnetic states. This implies that the short-range correlation grows with decreasing temperature and leads to the zigzag AFM ordering at T < TN. The present study provides a comprehensive picture of the magnetic correlations over the temperature range above and below TN and their relation to the crystal structure. The role of intermediate soft Na-layers on the magnetic coupling between honeycomb planes is discussed.

cond-mat.str-el↗

arXiv2016

Long-range and short-range magnetic correlations, and microscopic origin of net magnetization in the spin-1 trimer chain compound CaNi3P4O14

Spin-spin correlations and microscopic origin of net magnetization in the spin-1 trimer chain compound CaNi3P4O14 have been investigated by powder neutron diffraction. The present study reveals a 3D long-range magnetic ordering below 16 K where the magnetic structure consists of ferromagnetic trimers that are coupled ferromagnetically along the spin-chain. The moment components along the a and c axes arrange antiferromagnetically. Our study establishes that the uncompensated moment components along the b axis result in a net magnetization per unit cell. The magnetic structure, determined in the present study, is in agreement with the results of recent first principles calculation; however, it is in contrast to a fascinating experimental prediction of ferrimagnetic ordering based on the periodicity of the exchange interactions in CaNi3P4O14. Our study also confirms the presence of broad diffuse magnetic scattering, due to 1D short-range spin-spin correlations, over a wide temperature range below ~50 K down to a temperature well below the Tc. Total neutron scattering analysis by the RMC method reveals that the dominating spin-spin correlation above Tc is ferromagnetic and along the b axis. The nearest neighbour spin-spin correlations along the a and c axes are found to be weakly antiferromagnetic. The nature of the trimer spin structure of the short-range state is similar to that of the 3D long-range ordered state. The present investigation of microscopic nature of the magnetic ground state also explains the condition required for the 1/3 magnetization plateau to be observed in the trimer spin-chains. In spite of the S=1 trimer chain system, the present compound CaNi3P4O14 is found to be a good realization of 3D magnet below the Tc=16 K with full ordered moment values of ~2 mu_B/Ni2+ (1.98 and 1.96 mu_B/Ni2+ for two Ni sites, respectively) at 1.5 K.

cond-mat.str-el↗