| 1. |
- Thota, S., et al.
(author)
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Unraveling the nature of ferrimagnetism and associated exchange interactions in distorted honeycomb Ni4Nb2O9
- 2022
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In: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 106:13
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Journal article (peer-reviewed)abstract
- Ferrimagnetism in orthorhombic Ni4Nb2O9 below its Neel temperature, T-FN similar to 76K is reported to result from two inequivalent Ni2+ ions having different magnetic moments. However, a clear understanding of the temperature variation of its magnetization [M(T)] for T > T-FN and T < T-FN in terms of a single set of exchange parameters is still lacking. In this work, experimental results obtained from a detailed analysis of the temperature and magnetic field dependence of magnetization [M(T, H)], ac-magnetic susceptibility [chi(ac)( f, T, H)], and heat-capacity [C-P(T, H)] measurements are combined with theoretical analysis to provide new insights into the nature of ferrimagnetism in Ni4Nb2O9. X-ray diffraction/Rietveld analysis of the prepared sample yielded the structural parameters of the orthorhombic crystal in agreement with previous studies, whereas x-ray photoelectron spectroscopy confirmed the Ni2+ and Nb5+ electronic states in Ni4Nb2O9. Analysis of chi(ac)(T) shows the paramagnetic-to-ferrimagnetic transition occurs at 76.5 K (T-FN), which increases with applied field H as T-FN proportional to H-0.35 due to the coupling of the ferromagnetic component with H. For T > T-FN, the chi(dc) versus T data are fitted to the Neel's expression for ferrimagnets, yielding the g-factors for the two Ni2+ ions as g(A) = 2.47 and g(B) = 2.10. Also, the antiferromagnetic molecular field constants between the A and B sublattices were evaluated as N-AA = 26.31, N-BB = 8.59, and N-AB = 43.06, which, in turn, yield the antiferromagnetic exchange parameters: J(AA)/k(B) = 4.27 K, J(BB)/k(B) = 1.40 K, and J(AB)/k(B) = 6.98 K. For T < T-FN, the M versus T data clearly show the magnetic compensation point at T-COM similar to 33 K. The mathematical model presented here using the magnitudes of NAA, NBB, and NAB correctly predicts the position of T-COM as well the temperature variation of M both above and below T-COM. The data of C-P(T) versus T shows a lambda-type anomaly across T-FN. After subtracting the lattice contribution, the C-P(T) data are fitted to C-P = A(T - T-N)((-alpha)) yielding the critical exponent alpha = 0.14(0.12) for T < T-FN (T > T-FN), which is a characteristic of second-order phase transition. Magnetic entropy changes determined from the M-H isotherms shows that the applied field H enhances the magnetic ordering for T > T-FN and T < T-COM, but for T-COM < T < T-FN, the spin disorder increases with the increase in H. The temperature variation of the measured coercivity H-C(T) and remanence M-R(T) from 1.9 K to T-FN initially show a decreasing trend, becoming zero at T-COM, then followed by an increase and eventually becoming zero again at T-FN.
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| 2. |
- Jena, S. K., et al.
(author)
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Spin-liquid state with precursor ferromagnetic clusters interacting antiferromagnetically in frustrated glassy tetragonal spinel Zn0.8Cu0.2FeMnO4
- 2023
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In: Journal of Physics. - : IOP Publishing. - 0953-8984 .- 1361-648X. ; 35:37
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Journal article (peer-reviewed)abstract
- Spinels (AB(2)O(4)) with magnetic ions occupying only the octahedral B sites have inherent magnetic frustration which inhibits magnetic long-range order (LRO) but may lead to exotic states. Here we report on the magnetic properties of the tetragonal spinel Zn0.8Cu0.2FeMnO4, the tetragonality resulting from the Jahn-Teller active Mn3+ ions. X-ray diffraction and x-ray photoelectron spectroscopy of the sample yielded the composition (Zn-0.8(2+) Cu-0.2(2+)) A [Fe-0.4(2+) Fe-0.6(3+) Mn3+](B)O4-delta. Analysis of the temperature dependence of magnetization (M), ac magnetic susceptibilities (chi' and chi''), dc susceptibility (chi), heat capacity C-p, and neutron diffraction (ND) measurements show complex temperature-dependent short-range order (SRO) but without LRO. The data of chi vs. T fits the Curie-Weiss law: chi = C/(T - theta) from T = 250 K to 400 K with theta similar or equal to 185 K signifying dominant ferromagnetic (FM) coupling with the FM exchange constant J/k(B) = 17 K, and C = 3.29 emu K mol(-1) Oe(-1) yielding an effective magnetic moment mu(eff) = 5.13 mu B resulting from the high-spin states of Cu2+ (A site) and Fe2+ (B site), while the B site trivalent ions Mn3+ and Fe3+ are in their low-spin states. The extrapolated saturation magnetization obtained from the M vs. H data at T = 2 K is explained using the spin arrangement (Cu2+down arrow)(A)[Fe2+down arrow, Fe3+down arrow, Mn3+down arrow](B) leading to FM clusters interact antiferromagnetically at low temperatures. Temperature dependence of d(chi T)/ dT shows the onset of ferrimagnetism below similar to 100 K and peaks near 47 K and 24 K. The relaxation time t obtained from temperature and frequency dependence of chi'' when fit to the power law and Vogel-Fulcher laws confirm the cluster spin-glass (SG) state. The magnetic field dependence of the SG temperature T-SG (H) follows the equation: T-SG (H) = T-SG (0) [ 1- AH(2/phi)] with T-SG (0) = 46.6 K, A = 8.6 x 10(-3) Oe(-0.593) and phi = 3.37. The temperature dependence of hysteresis loops yields coercivity H-C similar to 3.8 kOe at 2 K without exchange-bias, but HC decreases with increase in T becoming zero above 24 K, the T-SG(H) for H = 800 Oe. Variations of C-p vs. T from 2 K to 200 K in H = 0 and H = 90 kOe do not show any peak characteristic of LRO. However, after correcting for the lattice contribution, a broad weak peak typically of SRO becomes evident centered around 40 K. For T < 9 K, Cp varies as T-2; a typical signature of spin-liquids (SLs). Comparison of the ND measurements at 1.7 K and 79.4 K shows absence of LRO. Time dependence of thermo-remanent magnetization MTRM(t) studies below 9 K reveal weakening of the inter-cluster interaction with increase in temperature. A summary of these results is that in Zn0.8Cu0.2FeMnO4, ferromagnetic clusters interact antiferromagnetically without LRO but producing a cluster SG state at T-SG(0) = 46.6 K, followed by SL behavior below 9 K.
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| 3. |
- Singha, A. D., et al.
(author)
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Reentrant canonical spin-glass dynamics and tunable field-induced transitions in (GeMn)Co2O4 Kagomé lattice
- 2024
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In: Journal of Physics. - : Institute of Physics Publishing (IOPP). - 0953-8984 .- 1361-648X. ; 36:7
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Journal article (peer-reviewed)abstract
- We report on the reentrant canonical semi spin-glass characteristics and controllable field-induced transitions in distorted Kagomé symmetry of (GeMn)Co2O4. This B-site spinel exhibits complicated, yet interesting magnetic behaviour in which the longitudinal ferrimagnetic (FiM) order sets in below the Néel temperature TFN ∼ 77 K due to uneven moments of divalent Co (↑ 5.33 μB) and tetravalent Mn (↓ 3.87 μB) which coexists with transverse spin-glass state below 72.85 K. Such complicated magnetic behaviour is suggested to result from the competing anisotropic superexchange interactions (JAB/kB ∼ 4.3 K, JAA/kB ∼ −6.2 K and JBB/kB ∼ −3.3 K) between the cations, which is extracted following the Néel's expression for the two-sublattice model of FiM. Dynamical susceptibility (χac (f, T)) and relaxation of thermoremanent magnetization, MTRM (t) data have been analysed by means of the empirical scaling-laws such as Vogel–Fulcher law and Power law of critical slowing down. Both of which reveal the reentrant spin-glass like character which evolves through a number of intermediate metastable states. The magnitude of Mydosh parameter (Ω ∼ 0.002), critical exponent zυ = (6.7 ± 0.07), spin relaxation time τ0 = (2.33 ± 0.1) × 10−18 s, activation energy Ea/kB = (69.8 ± 0.95) K and interparticle interaction strength (T0 = 71.6 K) provide the experimental evidences for canonical spin-glass state below the spin freezing temperature TF = 72.85 K. The field dependence of TF obtained from χac (T) follows the irreversibility in terms of de Almeida–Thouless mean-field instability in which the magnitude of crossover scaling exponent Φ turns out to be ∼2.9 for the (Ge0.8Mn0.2)Co2O4. Isothermal magnetization plots reveal two field-induced transitions across 9.52 kOe (HSF1) and 45.6 kOe (HSF2) associated with the FiM domains and spin-flip transition, respectively. Analysis of the inverse paramagnetic susceptibility after subtracting the temperature independent diamagnetic term (=−3 × 10−3 emu mol−1 Oe−1) results in the effective magnetic moment = 7.654 μB/f.u. This agrees well with the theoretically obtained = 7.58 μB/f.u. resulting the cation distribution in support of the Hund's ground state spin configuration and of Mn4+ and Co2+, respectively. The H–T phase diagram has been established by analysing all the parameters (TF(H), TFN(H), HSF1(T) and HSF2(T)) extracted from various magnetization measurements. This diagram enables clear differentiation among the different phases of the (GeMn)Co2O4 and also illustrates the demarcation between short-range and long-range ordered regions.
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| 4. |
- Pramanik, Prativa, et al.
(author)
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Interplay of lattice-spin-orbital coupling and Jahn-Teller effect in noncollinear spinel Ti x Mn1-x (Fe y Co1-y )2O4 : a neutron diffraction study
- 2024
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In: Journal of Physics. - : Institute of Physics (IOP). - 0953-8984 .- 1361-648X. ; 36:35
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Journal article (peer-reviewed)abstract
- Local magnetostructural changes and dynamical spin fluctuations in doubly diluted spinel TixMn1-x(FeyCo1-y)(2)O-4 has been reported by means of neutron diffraction and magnetization studies. Two distinct sets of compositions (i) x(Ti) = 0.20 and y(Fe) = 0.18; (ii) x(Ti) = 0.40 and y(Fe) = 0.435 have been considered for this study. The first compound of equivalent stoichiometry Ti0.20Mn0.80Fe0.36Co1.64O4 exhibits enhanced tetragonal distortion across the ferrimagnetic transition temperature T-C = 258 K in comparison to the end compound MnCo2O4 (T-C similar to 180 K) with a characteristic ratio c(t)/root 2a(t) of 0.99795(8) demonstrating robust lattice-spin-orbital coupling. However, in the second case Ti0.40Mn0.60Fe0.87Co1.13O4 with higher B-site compositions, the presence of Jahn-Teller ions with distinct behavior appears to counterbalance the strong tetragonal distortion thereby ceasing the lattice-spin-orbital coupling. Both the investigated systems show the coexistence of noncollinear antiferromagnetic and ferrimagnetic components in cubic and tetragonal settings. On the other hand, the dynamical ac-susceptibility, chi(ac)(T) reveals a cluster spin-glass state with Gabay-Toulouse (GT) like mixed phases behaviour below T-C. Such dispersive behaviour appears to be sensitive to the level of octahedral substitution. Further, the field dependence of chi(ac)(T) follows the weak anisotropic GT-line behaviour with crossover exponent Phi lies in the range 1.38-1.52 on the H-T plane which is in contrast to the B-site Ti substituted MnCo2O4 spinel that appears to follow irreversible non-mean-field AT-line behaviour (Phi similar to 3 + delta). Finally, the Arrott plots analysis indicates the presence of a pseudo first-order like transition (T < 20 K) which is in consonance with and zero crossover of the magnetic entropy change within the frozen spin-glass regime.
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| 5. |
- Pramanik, P., et al.
(author)
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Neutron diffraction evidence for local spin canting, weak Jahn-Teller distortion, and magnetic compensation in Ti1-xMnxCo2O4 spinel
- 2020
-
In: Journal of Physics. - : IOP PUBLISHING LTD. - 0953-8984 .- 1361-648X. ; 32:24
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Journal article (peer-reviewed)abstract
- A systematic study using neutron diffraction and magnetic susceptibility is reported on Mn substituted ferrimagnetic inverse spinel Ti1-xMnxCo2O4 in the temperature interval 1.6 K T 300 K. Our neutron diffraction study reveals cooperative distortions of the TO6 octahedra in the Ti1-xMnxCo2O4 system for all the Jahn-Teller active ions T = Mn3+ , Ti3+ and Co3+ , having the electronic configurations 3d(1), 3d(4) and 3d(6), respectively which are confirmed by the x-ray photoelectron spectroscopy. Two specific compositions (x = 0.2 and 0.4) have been chosen in this study because these two systems show unique features such as; (i) noncollinear Yafet-Kittel type magnetic ordering, and (ii) weak tetragonal distortion with c/a < 1, in which the apical bond length d(c)(T-B-O) is longer than the equatorial bond length d(ab)(T-B-O) due to the splitting of the e(g) level of Mn3+ ions into and . For the composition x = 0.4, the distortion in the TBO6 octahedra is stronger as compared to x = 0.2 because of the higher content of trivalent Mn. Ferrimagnetic ordering in Ti0.6Mn0.4Co2O4 and Ti0.8Mn0.2Co2O4 sets in at 110.3 and 78.2 K, respectively due to the presence of unequal magnetic moments of cations, where Ti3+ , Mn3+ , and Co3+ occupy the octahedral, whereas, Co2+ sits in the tetrahedral site. For both compounds an additional weak antiferromagnetic component could be observed lying perpendicular to the ferrimagnetic component. The analysis of static and dynamic magnetic susceptibilities combined with the heat-capacity data reveals a magnetic compensation phenomenon (MCP) at T-COMP = 25.4 K in Ti0.8Mn0.2Co2O4 and a reentrant spin-glass behaviour in Ti0.6Mn0.4Co2O4 with a freezing temperature of 110.1 K. The MCP in this compound is characterized by sign reversal of magnetization and bipolar exchange bias effect below T-COMP with its magnitude depending on the direction of external magnetic field and the cooling protocol.
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| 6. |
- Yuan, J., et al.
(author)
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Elevated plasma sclerostin is associated with high brain amyloid-β load in cognitively normal older adults
- 2023
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In: Npj Aging. - 2731-6068. ; 9:1
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Journal article (peer-reviewed)abstract
- Osteoporosis and Alzheimer's disease (AD) mainly affect older individuals, and the possibility of an underlying link contributing to their shared epidemiological features has rarely been investigated. In the current study, we investigated the association between levels of plasma sclerostin (SOST), a protein primarily produced by bone, and brain amyloid-beta (A ss) load, a pathological hallmark of AD. The study enrolled participants meeting a set of screening inclusion and exclusion criteria and were stratified into A ss(n = 65) and A ss+ (n = 35) according to their brain A ss load assessed using A ss-PET (positron emission tomography) imaging. Plasma SOST levels, apolipoprotein E gene (APOE) genotype and several putative AD blood-biomarkers including A ss 40, A ss 42, A ss 42/A ss 40, neurofilament light (NFL), glial fibrillary acidic protein (GFAP), total tau (t-tau) and phosphorylated tau (p-tau181 and p-tau231) were detected and compared. It was found that plasma SOST levels were significantly higher in the A ss+ group (71.49 +/- 25.00 pmol/L) compared with the A ss- group (56.51 +/- 22.14 pmol/L) (P < 0.01). Moreover, Spearman's correlation analysis showed that plasma SOST concentrations were positively correlated with brain A ss load (. = 0.321, P = 0.001). Importantly, plasma SOST combined with A ss 42/A ss 40 ratio significantly increased the area under the curve (AUC) when compared with using A ss 42/A ss 40 ratio alone (AUC = 0.768 vs 0.669, P = 0.027). In conclusion, plasma SOST levels are elevated in cognitively unimpaired older adults at high risk of AD and SOST could complement existing plasma biomarkers to assist in the detection of preclinical AD.
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| 7. |
- Chowdhury, Mouli Roy, et al.
(author)
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Antiferromagnetic short-range order and cluster spin-glass state in diluted spinel ZnTiCoO4
- 2022
-
In: Journal of Physics. - : IOP Publishing Ltd. - 0953-8984 .- 1361-648X. ; 34:27
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Journal article (peer-reviewed)abstract
- The nature of magnetism in the doubly-diluted spinel ZnTiCoO4 = (Zn2+)( A ) [Ti4+Co2+]( B )O-4 is reported here employing the temperature and magnetic field (H) dependence of dc susceptibility (chi), ac susceptibilities (chi ' and chi ''), and heat capacity (C (p)) measurements. Whereas antiferromagnetic (AFM) Neel temperature T (N) = 13.9 K is determined from the peak in the partial differential (chi T)/ partial differential T vs T plot, the fit of the relaxation time tau (determined from the peak in the chi '' vs T data at different frequencies) to the Power law: tau = tau (0) [(T - T (SG))/T (SG)](-z nu ) yields the spin glass freezing temperature T (SG) = 12.9 K, z nu similar to 11.75, and tau (0) similar to 10(-12) s. Since the magnitudes of tau (0) and z nu depend on the magnitude of T (SG), a procedure is developed to find the optimum value of T (SG) = 12.9 K. A similar procedure is used to determine the optimum T (0) = 10.9 K in the Vogel-Fulcher law: tau = tau (0) exp[E (a)/k (B)(T - T (0))] yielding E (a)/k (B) = 95 K, and tau (0) = 1.6 x 10(-13) s. It is argued that the comparatively large magnitude of the Mydosh parameter omega = 0.026 and k (B) T (0)/E (a) = 0.115 (MUCH LESS-THAN1) suggests cluster spin-glass state in ZnTiCoO4 below T-SG. In the C (p) vs T data from 1.9 K to 50 K, only a broad peak near 20 K is observed. This and absence of lambda-type anomaly near T (N) or T (SG) combined with the reduced value of change in magnetic entropy from 50 K to 1.9 K suggests only short-range AFM ordering in the system, consistent with spin-glass state. The field dependence of T (SG) shows slight departure (phi similar to 4.0) from the non-mean-field Almeida-Thouless line T (SG)(H) = T (SG)(0) (1 - AH (2/phi )). Strong temperature dependence of magnetic viscosity S and coercivity H (C) without exchange bias, both tending to zero on approach to T (SG) from below, further support the spin-glass state which results from magnetic dilution driven by diamagnetic Zn2+ and Ti4+ ions leading to magnetic frustration. Magnetic phase diagram in the H-T plane is established using the high-field magnetization data M(H, T) for T < T (N) which reveals rapid decrease of T (SG) with increase in H whereas decrease in T (N) with increase in H is weaker, typical of AFM systems. For T > T (N), the data of chi vs T are fit to the modified Curie-Weiss law, chi = chi (0) + C/(T + theta), with chi (0) = 3.2 x 10(-4) emu mol(-1) Oe(-1) yielding theta = 4 K and C = 2.70 emu K mol(-1) Oe(-1). This magnitude of C yields effective magnetic moment = 4.65 mu (B) for Co2+, characteristic of Co2+ ions with some contribution from spin-orbit coupling. Molecular field theory with effective spin S = 3/2 of Co2+ is used to determine the nearest-neighbor exchange constant J (1)/k (B) = 2. 39 K AFM and next-nearest-neighbor exchange constant J (2)/k (B) = -0.66 K (ferromagnetic).
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| 8. |
- Ghosh, Sayandeep, et al.
(author)
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Antiferromagnetism, spin-glass state, H-T phase diagram, and inverse magnetocaloric effect in Co2RuO4
- 2020
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In: Journal of Physics. - : IOP Publishing. - 0953-8984 .- 1361-648X. ; 32:48
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Journal article (peer-reviewed)abstract
- Static and dynamic magnetic properties of normal spinel Co2RuO4= (Co2+)A[Co3+Ru3+](B)O-4 are reported based on our investigations of the temperature (T), magnetic field (H) and frequency (f) dependence of the ac-magnetic susceptibilities and dc-magnetization (M) covering the temperature rangeT= 2 K-400 K and H up to 90 kOe. These investigations show that Co2RuO4 exhibits an antiferromagnetic (AFM) transition at T-N similar to 15.2 K, along with a spin-glass state at slightly lower temperature (T-SG) near 14.2 K. It is argued thatT(N)is mainly governed by the ordering of the spins of Co2+ ions occupying theA-site, whereas the exchange interaction between the Co2+ ions on theA-site and randomly distributed Ru(3+)on theB-site triggers the spin-glass phase, Co3+ ions on theB-site being in the low-spin non-magnetic state. Analysis of measurements ofM(H,T) for TT-N, analysis of the paramagnetic susceptibility (chi) vs.Tdata are fit to the modified Curie-Weiss law,chi=chi(0)+C/(T+theta), with chi(0)= 0.0015 emu mol(-1)Oe(-1)yielding theta= 53 K andC= 2.16 emu-K mol(-1)Oe(-1), the later yielding an effective magnetic moment mu(eff)= 4.16 mu(B)comparable to the expected value of mu(eff)= 4.24 mu(B)per Co2RuO4. Using T-N,theta and high temperature series for chi, dominant exchange constant J(1)/k(B)similar to 6 K between the Co(2+)on theA-sites is estimated. Analysis of the ac magnetic susceptibilities near T-SG yields the dynamical critical exponent z nu= 5.2 and microscopic spin relaxation time tau(0)similar to 1.16 x 10(-10)sec characteristic of cluster spin-glasses and the observed time-dependence ofM(t) is supportive of the spin-glass state. LargeM-Hloop asymmetry at low temperatures with giant exchange bias effect (H-EB similar to 1.8 kOe) and coercivity (H-C similar to 7 kOe) for a field cooled sample further support the mixed magnetic phase nature of this interesting spinel. The negative magnetocaloric effect observed belowT(N)is interpreted to be due to the AFM and SG ordering. It is argued that the observed change from positive MCE (magnetocaloric effect) forT>T(N)to inverse MCE forT
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