Search

By means of single-crystal X-ray diffraction we have revealed the breaking of centrosymmetry when lowering the temperature under T$_s$ = 200 K concomitantly with the setting of a commensurate superstructure in the small A-site quadruple perovskite YMn$_3$Mn$_4$O$_{12}$. This results is in agreement with all data already reported for this compounds and solve the previous inconsistency about the Yttrium position. The superstructure is characterized by the appearing of satellite reflections in the single crystal pattern, consistent with an I-centered pseudo-orthorhombic commensurate supercell with $a \approx \sqrt{a_F} = 10.4352(7)$ \AA, $b \approx 2b_F = 14.6049(9)$ \AA, $c \approx \sqrt{c_F} = 10.6961(7)$ \AA and $\beta = 90.110(3)^\circ$, where F stands for the "fundamental" high-temperature cell ($a_F \approx c_F \approx 7.45$ \AA, $b_F \approx 7.34$ \AA, and $\beta \approx 90^\circ$). The space-group was unequivocally found to be Ia, which is non polar, thus allowing for a non-zero polarization in the material. We then have investigated in detail the pyrocurrent, transport, dielectric and the DC and AC magnetic properties of polycrystalline sample of YMn$_3$Mn$_4$O$_{12}$ over a wide temperature range. These measurements clearly highlight several critical temperatures in the material and correlation between the different orders: i) the centrosymmetry is broken at high temperature (T$_S$ = 200K), ii) then the long-range magnetic order of B-sites occurs at T$_{N,B}$ = 108 K and at this same temperature the compound enters in an insulating dielectric state. iii) Finally, a remnant polarization is stabilized concomitantly with a magnetic anomaly at T* = 70 K. We propose that YMn$_3$Mn$_4$O$_{12}$ is a peculiar magnetic ferroelectric in which the polar state is driven by short-range magnetic order.

We investigate the specific influence of structural disorder on the suppression of antiferromagnetic order and on the emergence of cuprate superconductivity. We single out pure disorder, by focusing on a series of Y$_{z}$Eu$_{1-z}$Ba$_2$Cu$_3$O$_{6+y}$ samples at fixed oxygen content $y=0.35$, in the range $0\le z\le 1$. The gradual Y/Eu isovalent substitution smoothly drives the system through the Mott-insulator to superconductor transition from a full antiferromagnet with N\'eel transition $T_N=320$ K at $z=0$ to a bulk superconductor with superconducting critical temperature $T_c=18$ K at $z=1$, YBa$_2$Cu$_3$O$_{6.35}$. The electronic properties are finely tuned by gradual lattice deformations induced by the different cationic radii of the two lanthanides, inducing a continuous change of the basal Cu(1)-O chain length, as well as a controlled amount of disorder in the active Cu(2)O$_2$ bilayers. We check that internal charge transfer from the basal to the active plane is entirely responsible for the doping of the latter and we show that superconductivity emerges with orthorhombicity. By comparing transition temperatures with those of the isoelectronic clean system we deterime the influence of pure structural disorder connected with the Y/Eu alloy., Comment: 10 pages 11 figures, submitted to Journal of Physics: Condensed Matter, Special Issue in memory of Prof. Sandro Massida

BiMnO3 (BMO), ferromagnetic (FM) below Tc = 100 K, was believed to be also ferroelectric (FE) due to a non-centro-symmetric C2 structure, until diffraction data indicated that its space group is the centro-symmetric C2/c. Here we present infrared phonon spectra of BMO, taken on a mosaic of single crystals, which are consistent with C2/c at any T > 10 K, as well as room-temperature Raman data which strongly support this conclusion. We also find that the infrared intensity of several phonons increases steadily for decreasing T, causing the relative permittivity of BMO to vary from 18.5 at 300 K to 45 at 10 K. At variance with FE materials of displacive type, no appreciable softening has been found in the infrared phonons. Both their frequencies and intensities, moreover, appear insensitive to the FM transition at Tc.

We report on a systematic study of the structural, magnetic and transport properties of high-purity 1T-VS$_2$ powder samples prepared under high pressure. The results differ notably from those previously obtained by de-intercalating Li from LiVS$_2$. First, no Charge Density Wave (CDW) is found by transmission electron microscopy down to 94 K. Though, \textit{ab initio} phonon calculations unveil a latent CDW instability driven by an acoustic phonon softening at the wave vector ${\bf q}_{CDW} \approx$ (0.21,0.21,0) previously reported in de-intercalated samples. A further indication of latent lattice instability is given by an anomalous expansion of the V-S bond distance at low temperature. Second, infrared optical absorption and electrical resistivity measurements give evidence of non metallic properties, consistent with the observation of no CDW phase. On the other hand, magnetic susceptibility and NMR data suggest the coexistence of localized moments with metallic carriers, in agreement with \textit{ab initio} band structure calculations. This discrepancy is reconciled by a picture of electron localization induced by disorder or electronic correlations leading to a phase separation of metallic and non-metallic domains in the nm scale. We conclude that 1T-VS$_2$ is at the verge of a CDW transition and suggest that residual electronic doping in Li de-intercalated samples stabilizes a uniform CDW phase with metallic properties., Comment: 22 pages, 10 Figures. Full resolution pictures available at http://journals.aps.org/prb/abstract/10.1103/PhysRevB.89.235125

We report on an a $\mu$SR and $^{55}$Mn NMR investigation of the magnetic order parameter as a function of temperature in the optimally doped La$_{5/8}$(Ca$_y$Sr$_{1-y}$)$_{3/8}$MnO$_3$ and in the underdoped La$_{1-x}$Sr$_{x}$MnO$_3$ and La$_{1-x}$Ca$_{x}$MnO$_3$ metallic manganite families. The study is aimed at unraveling the effect of lattice distortions, implicitly controlled by the Ca-Sr isoelectronic substitution, from that of hole doping $x$ on the Curie temperature $T_c$ and the order of the magnetic transition. At optimal doping, the transitions are second order at all $y$ values, including the $y=1$ (La$_{5/8}$Ca$_{3/8}$MnO$_3$) end member. In contrast, they are first order in the underdoped samples, which show a finite (truncated) order parameter at the Curie point, including La$_{0.75}$Sr$_{0.25}$MnO$_3$ whose $T_c$ is much higher than that of La$_{5/8}$Ca$_{3/8}$MnO$_3$. The order parameter curves, on the other hand, exhibit a very minor dependence on $x$, if truncation is excepted. This suggests that the effective exchange interaction between Mn ions is essentially governed by local distortions, in agreement with the original double-exchange model, while truncation is primarily, if not entirely, an effect of under- or overdoping. A phase diagram, separating in the $x-y$ plane polaron-driven first order transitions from regular second order transitions governed by critical fluctuations, is proposed for the La$_{1-x}($Ca$_y$Sr$_{1-y}$)$_{x}$MnO$_3$ system., Comment: submitted to Phys. Rev. B

By means of neutron powder diffraction, we investigated the effect of the polar Bi$^{3+}$ ion on the magnetic ordering of the Mn$^{3+}$ ions in BiMn$_3$Mn$_4$O$_{12}$, the counterpart with \textit{quadruple} perovskite structure of the \textit{simple} perovskite BiMnO$_3$. The data are consistent with a \textit{noncentrosymmetric} spacegroup $Im$ which contrasts the \textit{centrosymmetric} one $I2/m$ previously reported for the isovalent and isomorphic compound LaMn$_3$Mn$_4$O$_{12}$, which gives evidence of a Bi$^{3+}$-induced polarization of the lattice. At low temperature, the two Mn$^{3+}$ sublattices of the $A'$ and $B$ sites order antiferromagnetically (AFM) in an independent manner at 25 and 55 K, similarly to the case of LaMn$_3$Mn$_4$O$_{12}$. However, both magnetic structures of BiMn$_3$Mn$_4$O$_{12}$ radically differ from those of LaMn$_3$Mn$_4$O$_{12}$. In BiMn$_3$Mn$_4$O$_{12}$ the moments $\textbf{M}_{A'}$ of the $A'$ sites form an anti-body AFM structure, whilst the moments \textbf{M}$_{B}$ of the $B$ sites result from a large and \textit{uniform} modulation $\pm \textbf{M}_{B,b}$ along the b-axis of the moments \textbf{M}$_{B,ac}$ in the $ac$-plane. The modulation is strikingly correlated with the displacements of the Mn$^{3+}$ ions induced by the Bi$^{3+}$ ions. Our analysis unveils a strong magnetoelastic coupling between the internal strain created by the Bi$^{3+}$ ions and the moment of the Mn$^{3+}$ ions in the $B$ sites. This is ascribed to the high symmetry of the oxygen sites and to the absence of oxygen defects, two characteristics of quadruple perovskites not found in simple ones, which prevent the release of the Bi$^{3+}$-induced strain through distortions or disorder. This demonstrates the possibility of a large magnetoelectric coupling in proper ferroelectrics and suggests a novel concept of internal strain engineering for multiferroics design., Comment: 9 pages, 7 figures, 5 tables

We report on the high pressure synthesis of BiMn$_7$O$_{12}$, a manganite displaying a "quadruple perovskite" structure. Structural characterization of single crystal samples shows a distorted and asymmetrical coordination around the Bi atom, due to presence of the $6s^{2}$ lone pair, resulting in non-centrosymmetric space group Im, leading to a permanent electrical dipole moment and ferroelectric properties. On the other hand, magnetic characterization reveals antiferromagnetic transitions, in agreement with the isostructural compounds, thus evidencing two intrinsic properties that make BiMn$_7$O$_{12}$ a promising multiferroic material., Comment: 4 pages, 3 figures

The structural properties of BiMn$O_3$ were determined from neutron powder diffraction data as a function of temperature and magnetic field. The structure at all temperatures was found to be centrosymmetric with space group $C2/c$, which is incompatible with ferroelectricity. At T$_C\simeq 100 K$, we observed the onset of a large magnetoelastic strain, proportional to the square of the magnetization. We interpret this structural rearrangement, together with the previously observed magnetodielectric anomalies, as due to the need to optimize the partially frustrated magnetic interactions., Comment: 4 pages, 4 figures

The oxygen-order dependent emergence of superconductivity in YBa2Cu3O6+x is studied, for the first time in a comparative way, on pair samples having the same oxygen content and thermal history, but different Cu(1)Ox chain arrangements deriving from their intercalated and deintercalated nature. Structural and electronic non-equivalence of pairs samples is detected in the critical region and found to be related, on microscopic scale, to a different average chain length, which, on being experimentally determined by nuclear quadrupole resonance (NQR), sheds new light on the concept of critical chain length for hole doping efficiency., Comment: 7 RevTex pages, 2 Postscript figures. Submitted to Phys. Rev. B

We report a study of polycrystalline samples of the family La1-xCdxMnO3+dwith different percentage of Mn4+ ions. X-rays diffraction, Iodometric titration, Raman, Magnetic and Electrical Resistivity measurements provide a general characterisation of the physical properties. Results are qualitatively similar to the ones found in Ca doped manganese perovskites. Key words: Cd, manganese perovskites, magnetoresistance, Raman, magnetic, resistivity, Comment: 7 pages including 3 figures