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Emergence of a correlated insulating state in bulk 1T-NbSe$_2$ via metal intercalation
Authors:
M. Tomlinson,
AKM A. Rahman,
S. Devi,
R. Tuchikawa,
M. Ishigami,
D. Le,
Md Z. Mohayman,
A. Kushima,
Y. Nakajima
Abstract:
The 1T polymorph of NbSe$_2$, long confined to the monolayer limit, has remained inaccessible in bulk. Here, we report the realization of bulk 1T-NbSe$_2$ via electrochemical Sn intercalation. Transmission electron microscopy directly reveals the formation of the 1T structure induced by Sn intercalation. The intercalated samples exhibit insulating transport behavior, in stark contrast to metallic…
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The 1T polymorph of NbSe$_2$, long confined to the monolayer limit, has remained inaccessible in bulk. Here, we report the realization of bulk 1T-NbSe$_2$ via electrochemical Sn intercalation. Transmission electron microscopy directly reveals the formation of the 1T structure induced by Sn intercalation. The intercalated samples exhibit insulating transport behavior, in stark contrast to metallic 2H-NbSe$_2$. Density functional theory calculations, however, predict a metallic band structure, highlighting the crucial role of emergent electronic correlations in the observed insulating state. Raman spectroscopy further reveals vibrational modes associated with Sn intercalation and possible charge density wave order. Our results establish electrochemical intercalation as an effective route to stabilize otherwise inaccessible bulk polytypes, positioning bulk 1T-NbSe$_2$ as a new platform for investigating correlated electronic states.
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Submitted 7 May, 2026;
originally announced May 2026.
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Data-Efficient Machine learning for Predicting Dopant Formation Energies in TiO$_2$ Monolayer
Authors:
Kati Asikainen,
Matti Alatalo,
Marko Huttula,
Assa Aravindh Sasikala Devi
Abstract:
Machine learning models are increasingly applied in materials science, yet their predictive power is often constrained by data scarcity. Here, we show that accurate predictions can be achieved, even with a limited number of training examples, provided the dataset is compact and and grounded in physically relevant quantities. By combining density functional theory calculations with a machine-learni…
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Machine learning models are increasingly applied in materials science, yet their predictive power is often constrained by data scarcity. Here, we show that accurate predictions can be achieved, even with a limited number of training examples, provided the dataset is compact and and grounded in physically relevant quantities. By combining density functional theory calculations with a machine-learning framework, we construct accurate descriptor-based models to predict the formation energies of doped lepidocrocite TiO$_2$ monolayers. The predictive accuracy of machine-learning models was first evaluated for single-dopant Pt configurations, demonstrating that the selected structural and chemical descriptors reliably capture the key factors governing dopant stability. Chemical transferability is then examined by extending the dataset to include Ag-doped configurations. Predictive accuracy improved systematically as additional Ag-doped data points were included in the training, while the performance of Pt remains robust. These results highlight the potential of small and well-curated datasets combined with physically informed descriptors to enable not only accurate but also chemically transferable machine-learning-driven screening in doped TiO$_2$ monolayer.
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Submitted 16 February, 2026;
originally announced February 2026.
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Investigating the Electronic and Magnetic Properties of Na$_x$Fe$_{1/2}$Mn$_{1/2}$O$_2$ Cathode Materials with X-ray Compton Scattering
Authors:
Veenavee Nipunika Kothalawala,
Kosuke Suzuki,
Johannes Nokelainen,
Ilja Makkonen,
Erica West,
Lassi Roininen,
Jere Leinonen,
Pekka Tynjälä,
Petteri Laine,
Juho Välikangas,
Ulla Lassi,
Assa Aravindh Sasikala Devi,
Matti Alatalo,
Yuki Mizuno,
Naruki Tsuji,
Hikaru Usami,
Yuju Nagasaki,
Tsuyoshi Takami,
Yoshiharu Sakurai,
Hiroshi Sakurai,
Mohammad Babar,
Venkat Vishwanathan,
Arun Bansil,
Bernardo Barbiellini
Abstract:
We discuss electronic and magnetic properties of Na$_x$Fe$_{1/2}$Mn$_{1/2}$O$_2$, a promising Na-ion battery cathode material. Using x-ray Compton scattering, SQUID magnetometry, and density-functional-theory based modeling, we probe how electrons and spins evolve during sodiation. By comparing Compton profiles of sodiated and desodiated samples, we show that oxygen 2$p$ orbitals drive the redox p…
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We discuss electronic and magnetic properties of Na$_x$Fe$_{1/2}$Mn$_{1/2}$O$_2$, a promising Na-ion battery cathode material. Using x-ray Compton scattering, SQUID magnetometry, and density-functional-theory based modeling, we probe how electrons and spins evolve during sodiation. By comparing Compton profiles of sodiated and desodiated samples, we show that oxygen 2$p$ orbitals drive the redox process, while transition-metal 3$d$ electrons become more delocalized, explaining the metallic phase at $x=2/3$. These profile differences define a quantitative descriptor for the sodiation range associated with improved conductivity. Electron holes on oxygen, reflected in oxygen magnetization, confirm the important role of oxygen in the electrochemical activity of the cathode.
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Submitted 12 February, 2026;
originally announced February 2026.
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Coexistence of long-range magnetic order and dynamical magnetism in the V-based Kagome metals: A combined thermodynamic and $μ$SR study
Authors:
Sheetal Devi,
Yishui Zhou,
Thomas J. Hicken,
Zurab Guguchia,
Hubertus Luetkens,
Min-Kai Lee,
Lieh-Jeng Chang,
Yixi Su
Abstract:
V-based Kagome metals exhibit a unique lattice geometry that can give rise to exotic electronic and magnetic phenomena, making them an ideal platform to study the interplay of topology and magnetism. We present a combined thermodynamic and muon spin relaxation ($μ$SR) investigation of single-crystal RV$_{6}$Sn$_{6}$ (R = Tb, Dy, Ho, Er) compounds, focusing on their low-temperature magnetic behavio…
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V-based Kagome metals exhibit a unique lattice geometry that can give rise to exotic electronic and magnetic phenomena, making them an ideal platform to study the interplay of topology and magnetism. We present a combined thermodynamic and muon spin relaxation ($μ$SR) investigation of single-crystal RV$_{6}$Sn$_{6}$ (R = Tb, Dy, Ho, Er) compounds, focusing on their low-temperature magnetic behavior. Heat capacity and $μ$SR measurements reveal distinct magnetic phase transitions below 4 K, confirming the emergence of long-range magnetic order in all compounds studied. The $μ$SR results further indicate persistent spin fluctuations within the magnetically ordered state down to 50 mK, reflected in reduced ordered moments obtained from hyperfine analysis of the heat capacity measurements. These findings uncover the coexistence of static and dynamic magnetism in V-based Kagome metals and emphasizing the key role of 4$f$-electron anisotropy in shaping their magnetic ground states. Compared with the Mn-based RMn$_{6}$Sn$_{6}$ analogs, our results highlight the unique magnetism arising from the decoupled rare-earth sublattice and its interplay with the nonmagnetic V Kagome network.
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Submitted 13 January, 2026;
originally announced January 2026.
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Ground-state magnetic structures of topological kagome metals RV$_6$Sn$_6$ (R = Tb, Dy, Ho, Er)
Authors:
Yishui Zhou,
Min-Kai Lee,
Sabreen Hammouda,
Sheetal Devi,
Shin-Ichiro Yano,
Romain Sibille,
Oksana Zaharko,
Wolfgang Schmidt,
Karin Schmalzl,
Ketty Beauvois,
Eric Ressouche,
Po-Chun Chang,
Chun-Hao Huang,
Lieh-Jeng Chang,
Thomas Brückel,
Yixi Su
Abstract:
Magnetic kagome metals have attracted tremendous research interests recently, because they represent an ideal playground for exploring the fascinating interplay between their intrinsically inherited topologically non-trivial electron band structures, magnetism and electronic correlation effects, and the resultant novel electronic/magnetic states and emergent excitations. In this work, we report a…
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Magnetic kagome metals have attracted tremendous research interests recently, because they represent an ideal playground for exploring the fascinating interplay between their intrinsically inherited topologically non-trivial electron band structures, magnetism and electronic correlation effects, and the resultant novel electronic/magnetic states and emergent excitations. In this work, we report a comprehensive single-crystal neutron diffraction investigation of the ground-state magnetic structures of the recently discovered V-based topological kagome metals RV$_6$Sn$_6$ (R = Tb, Dy, Ho, Er). Furthermore, the sample synthesis details and our systematic studies of crystal structure, low-temperature magnetic and thermodynamic properties of these compounds via various in-house characterization techniques are also reported. It can be revealed that RV$_6$Sn$_6$ (R = Tb, Dy, Ho) have a collinear ferromagnetic order in the ground state, with the ordered magnetic moment aligned along the c axis for R = Tb, Ho, while approximately 20${^\circ}$ tilted off from the c axis for R = Dy. In contrast, ErV$_6$Sn$_6$ shows an A-type antiferromagnetic structure with a magnetic propagation vector k = (0, 0, 0.5), and with the ordered magnetic moment aligned in the ab plane. A comparison of the low-temperature magnetic structures for both the extensively investigated topological kagome metal series of RV$_6$Sn$_6$ and RMn$_6$Sn$_6$ is given in details. This allows to gain new insights into the complex magnetic interactions, diverse single-ion magnetic anisotropies and spin dynamics in these compounds. The reported ground-state magnetic structures in RV$_6$Sn$_6$ (R = Tb, Dy, Ho, Er) can pave the way for further explorations of the possible interplay between magnetism and topologically non-trivial electron band structures in the magnetically ordered phase regime.
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Submitted 21 November, 2024;
originally announced November 2024.
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Compton scattering study of strong orbital delocalization in a LiNiO$_2$ cathode
Authors:
Veenavee Nipunika Kothalawala,
Kosuke Suzuki,
Johannes Nokelainen,
Arttu Hyvönen,
Ilja Makkonen,
Bernardo Barbiellini,
Hasnain Hafiz,
Pekka Tynjälä,
Petteri Laine,
Juho Välikangas,
Tao Hu,
Ulla Lassi,
Kodai Takano,
Naruki Tsuji,
Yosuke Amada,
Assa Aravindh Sasikala Devi,
Matti Alatalo,
Yoshiharu Sakurai,
Hiroshi Sakurai,
Arun Bansil
Abstract:
Cobalt is used in Li-ion batteries, but it is expensive and could be replaced by nickel to deliver better performance at a lower cost. With this motivation, we discuss how the character of redox orbitals of LiNiO$_2$ can be ascertained through x-ray Compton scattering measurements combined with parallel first-principles simulations. Our analysis reveals the nature of hole states in Li-doped NiO re…
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Cobalt is used in Li-ion batteries, but it is expensive and could be replaced by nickel to deliver better performance at a lower cost. With this motivation, we discuss how the character of redox orbitals of LiNiO$_2$ can be ascertained through x-ray Compton scattering measurements combined with parallel first-principles simulations. Our analysis reveals the nature of hole states in Li-doped NiO resulting from the hybridization of O 2$p$ and Ni 3$d$ orbitals. Our study also gives insight into the ferromagnetic ground state and provides a pathway toward the rational design of next-generation battery materials.
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Submitted 22 January, 2024;
originally announced January 2024.
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Ab initio insights on the ultrafast strong-field dynamics of anatase TiO$_2$
Authors:
Sruthil Lal S. B,
Lokamani,
Kushal Ramakrishna,
Attila Cangi,
D Murali,
Matthias Posselt,
Assa Aravindh Sasikala Devi,
Alok Sharan
Abstract:
Electron dynamics of anatase TiO$_2$ under the influence of ultrashort and intense laser field is studied using the real-time time-dependent density functional theory (TDDFT). Our findings demonstrate the effectiveness of TDDFT calculations in modeling the electron dynamics of solids during ultrashort laser excitation, providing valuable insights for designing and optimizing nonlinear photonic dev…
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Electron dynamics of anatase TiO$_2$ under the influence of ultrashort and intense laser field is studied using the real-time time-dependent density functional theory (TDDFT). Our findings demonstrate the effectiveness of TDDFT calculations in modeling the electron dynamics of solids during ultrashort laser excitation, providing valuable insights for designing and optimizing nonlinear photonic devices. We analyze the perturbative and non-perturbative responses of TiO$_2$ to 30 fs laser pulses at 400 and 800 nm wavelengths, elucidating the underlying mechanisms. At 400 nm, ionization via single photon absorption dominates, even at very low intensities. At 800 nm, we observe ionization through two-photon absorption within the intensity range of $1\times10^{10}$ to $9\times10^{12}$ W/cm$^2$, with a transition from multiphoton to tunneling ionization occurring at $9\times10^{12}$ W/cm$^2$. We observe a sudden increase in energy and the number of excited electrons beyond $1\times10^{13}$ W/cm$^2$, leading to their saturation and subsequent laser-induced damage. We estimate the damage threshold of TiO$_2$ for 800 nm to be 0.1 J/cm$^2$. In the perturbative regime, induced currents exhibit a phase shift proportional to the peak intensity of the laser pulse. This phase shift is attributed to the intensity-dependent changes in the number of free carriers, indicative of the optical Kerr effect. Leveraging the linear dependence of phase shift on peak intensities, we estimate the nonlinear refractive index ($n_2$) of TiO$_2$ to be $3.54\times10^{-11}$ cm$^2$/W.
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Submitted 30 June, 2023;
originally announced June 2023.
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Quasiparticle electronic structure and optical response ($G_0W_0$+BSE) of anatase TiO$_2$ starting from modified HSE06 functionals
Authors:
Sruthil Lal S. B,
D Murali,
Matthias Posselt,
Assa Aravindh Sasikala Devi,
Alok Sharan
Abstract:
The quasiparticle electronic structure and optical excitation of anatase TiO$_2$ is determined within the framework of many-body perturbation theory (MBPT) by combining the $G_0W_0$ method and the Bethe-Salpeter Equation (BSE). A modified version of the HSE06 screened hybrid functional, that includes 20\% exact Fock exchange (HSE06(20)) as opposed to 25\% in the standard HSE06 functional, is used…
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The quasiparticle electronic structure and optical excitation of anatase TiO$_2$ is determined within the framework of many-body perturbation theory (MBPT) by combining the $G_0W_0$ method and the Bethe-Salpeter Equation (BSE). A modified version of the HSE06 screened hybrid functional, that includes 20\% exact Fock exchange (HSE06(20)) as opposed to 25\% in the standard HSE06 functional, is used to set up the starting Hamiltonian for $G_0W_0$+BSE calculations. The HSE06(20) functional accurately predicts the ground state electronic band structure. BSE calculations based on data from $G_0W_0$+HSE06(20) yield direct optical excitation energies and oscillator strengths in excellent agreement with existing experiments and theoretical calculations characterizing direct excitation. In particular, an exciton binding energy of 229 $\pm$ 10 meV is obtained, in close agreement with experiments. The projections of excitonic states onto the quasiparticle band structure in a fatband representation shows that the lowest optical transition of anatase TiO$_2$ consists of excitons originating from the mixing of direct transitions within band pairs running parallel to the $Γ-Z $ direction in the tetragonal Brillouin zone. This implies a strong spatial localization of excitons in the $xy$ plane of the lattice. This investigation highlights the importance of a suitable non-interacting Hamiltonian for the MBPT based quasiparticle $G_0W_0$ and subsequent BSE calculations and suggests HSE06(20) as an optimal choice in the case of anatase TiO$_2$.
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Submitted 1 December, 2021;
originally announced December 2021.
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Financial Market Dynamics: Superdiffusive or not?
Authors:
Sandhya Devi
Abstract:
The behavior of stock market returns over a period of 1-60 days has been investigated for S&P 500 and Nasdaq within the framework of nonextensive Tsallis statistics. Even for such long terms, the distributions of the returns are non-Gaussian. They have fat tails indicating that the stock returns do not follow a random walk model. In this work, a good fit to a Tsallis q-Gaussian distribution is obt…
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The behavior of stock market returns over a period of 1-60 days has been investigated for S&P 500 and Nasdaq within the framework of nonextensive Tsallis statistics. Even for such long terms, the distributions of the returns are non-Gaussian. They have fat tails indicating that the stock returns do not follow a random walk model. In this work, a good fit to a Tsallis q-Gaussian distribution is obtained for the distributions of all the returns using the method of Maximum Likelihood Estimate. For all the regions of data considered, the values of the scaling parameter q, estimated from one day returns, lie in the range 1.4 to 1.65. The estimated inverse mean square deviations (beta) show a power law behavior in time with exponent values between -0.91 and -1.1 indicating normal to mildly subdiffusive behavior. Quite often, the dynamics of market return distributions is modelled by a Fokker-Plank (FP) equation either with a linear drift and a nonlinear diffusion term or with just a nonlinear diffusion term. Both of these cases support a q-Gaussian distribution as a solution. The distributions obtained from current estimated parameters are compared with the solutions of the FP equations. For negligible drift term, the inverse mean square deviations (betaFP) from the FP model follow a power law with exponent values between -1.25 and -1.48 indicating superdiffusion. When the drift term is non-negligible, the corresponding betaFP do not follow a power law and become stationary after certain characteristic times that depend on the values of the drift parameter and q. Neither of these behaviors is supported by the results of the empirical fit.
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Submitted 14 September, 2017; v1 submitted 27 August, 2016;
originally announced August 2016.
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Electric and magnetic polarizabilities of hexagonal Ln2CuTiO6 (Ln=Y, Dy, Ho, Er and Yb)
Authors:
Debraj Choudhury,
Abhijit Hazarika,
Adyam Venimadhav,
Chandrasekhar Kakarla,
Kris T. Delaney,
P. Sujatha Devi,
P. Mondal,
R. Nirmala,
J. Gopalakrishnan,
Nicola A. Spaldin,
Umesh V. Waghmare,
D. D. Sarma
Abstract:
We investigated the rare-earth transition metal oxide series, Ln2CuTiO6 (Ln=Y, Dy, Ho, Er and Yb), crystallizing in the hexagonal structure with non-centrosymmetric P63cm space group for possible occurrences of multiferroic properties. Our results show that while these compounds, except Ln=Y, exhibit a low temperature antiferromagnetic transition due to the ordering of the rare-earth moments, the…
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We investigated the rare-earth transition metal oxide series, Ln2CuTiO6 (Ln=Y, Dy, Ho, Er and Yb), crystallizing in the hexagonal structure with non-centrosymmetric P63cm space group for possible occurrences of multiferroic properties. Our results show that while these compounds, except Ln=Y, exhibit a low temperature antiferromagnetic transition due to the ordering of the rare-earth moments, the expected ferroelectric transition is frustrated by the large size difference between Cu and Ti at the B-site. Interestingly, this leads these compounds to attain a rare and unique combination of desirable paraelectric properties with high dielectric constants, low losses and weak temperature and frequency dependencies. First-principles calculations establish these exceptional properties result from a combination of two effects. A significant difference in the MO5 polyhedral sizes for M = Cu and M = Ti suppress the expected co-operative tilt pattern of these polyhedra, required for the ferroelectric transition, leading to relatively large values of the dielectric constant for every compound investigated in this series. Additionally, it is shown that the majority contribution to the dielectric constant arises from intermediate-frequency polar vibrational modes, making it relatively stable against any temperature variation. Changes in the temperature stability of the dielectric constant amongst different members of this series are shown to arise from changes in relative contributions from soft polar modes.
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Submitted 24 September, 2010; v1 submitted 2 June, 2010;
originally announced June 2010.
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Correlation between extrinsic electroresistance and magnetoresistance in fine-grained La0.7Ca0.3MnO3
Authors:
P. Sujatha Devi,
A. Kumar,
Dipten Bhattacharya,
Shilpi Karmakar,
B. K. Chaudhuri
Abstract:
We report our observation of a correlation between the extrinsic electroresistance (EER) and magnetoresistance (EMR) via grain size in fine-grained La0.7Ca0.3MnO3. The nature of dependence of EER and EMR on grain size (~0.2-1.0 micron) indicates that for finer grains with low-resistive boundaries both of them follow similar trend whereas they differ for coarser grains with high-resistive boundarie…
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We report our observation of a correlation between the extrinsic electroresistance (EER) and magnetoresistance (EMR) via grain size in fine-grained La0.7Ca0.3MnO3. The nature of dependence of EER and EMR on grain size (~0.2-1.0 micron) indicates that for finer grains with low-resistive boundaries both of them follow similar trend whereas they differ for coarser grains with high-resistive boundaries. This could be due to a crossover in the mechanism of charge transport across the grain boundaries - from spin-depedent scattering process to spin-polarized tunneling one - as a function of grain size.
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Submitted 27 August, 2010; v1 submitted 22 August, 2008;
originally announced August 2008.
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Ferromagnetism in nanoscale BiFeO3
Authors:
R. Mazumder,
P. Sujatha Devi,
Dipten Bhattacharya,
P. Choudhury,
A. Sen,
M. Raja
Abstract:
A remarkably high saturation magnetization of ~0.4mu_B/Fe along with room temperature ferromagnetic hysteresis loop has been observed in nanoscale (4-40 nm) multiferroic BiFeO_3 which in bulk form exhibits weak magnetization (~0.02mu_B/Fe) and an antiferromagnetic order. The magnetic hysteresis loops, however, exhibit exchange bias as well as vertical asymmetry which could be because of spin pin…
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A remarkably high saturation magnetization of ~0.4mu_B/Fe along with room temperature ferromagnetic hysteresis loop has been observed in nanoscale (4-40 nm) multiferroic BiFeO_3 which in bulk form exhibits weak magnetization (~0.02mu_B/Fe) and an antiferromagnetic order. The magnetic hysteresis loops, however, exhibit exchange bias as well as vertical asymmetry which could be because of spin pinning at the boundaries between ferromagnetic and antiferromagnetic domains. Interestingly, like in bulk BiFeO_3, both the calorimetric and dielectric permittivity data in nanoscale BiFeO_3 exhibit characteristic features at the magnetic transition point. These features establish formation of a true ferromagnetic-ferroelectric system with a coupling between the respective order parameters in nanoscale BiFeO_3.
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Submitted 17 May, 2007;
originally announced May 2007.
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Orbital order-disorder transition in La(1-x)Nd(x)MnO(3) (x = 0.0-1.0) and La(1-x-y)Nd(yx)Sr(y)MnO(3) (x = 0.1; y = 0.05,0.1)
Authors:
Dipten Bhattacharya,
P. Sujatha Devi,
H. S. Maiti
Abstract:
The nature of orbital order-disorder transition has been studied in the La(1-x)Nd(x)MnO(3) (x = 0.0-1.0) series which covers the entire range between two end points - LaMnO(3) and NdMnO(3) - as well as in La(0.85)Nd(0.1)Sr(0.05)MnO(3) and La(0.8)Nd(0.1)Sr(0.1)MnO(3). It has been observed that the first-order nature of the transition gives way to higher order with the increase in "x" in the case…
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The nature of orbital order-disorder transition has been studied in the La(1-x)Nd(x)MnO(3) (x = 0.0-1.0) series which covers the entire range between two end points - LaMnO(3) and NdMnO(3) - as well as in La(0.85)Nd(0.1)Sr(0.05)MnO(3) and La(0.8)Nd(0.1)Sr(0.1)MnO(3). It has been observed that the first-order nature of the transition gives way to higher order with the increase in "x" in the case of pure manganites. The latent heat (L) associated with the transition, first, drops with a steeper slope within x = 0.0-0.3 and, then, gradually over a range 0.3<x<0.9. This drop could, possibly, be due to evolution of finer orbital domain structure with "x". In the case of Sr-doped samples, the transition appears to be of higher-order nature even for a doping level 5 at%. In both cases, of course, the transition temperature T(JT) rises systematically with the drop in average A-site radius <r(A)> or rise in average Mn-O-Mn bond bending angle <cos^2(phi)> while no apparent correlation could be observed with doping induced disorder sigma^2. The cooperative nature of the orbital order, therefore, appears to be robust.
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Submitted 7 December, 2004;
originally announced December 2004.