We have synthesized and characterized four different stable phases of Na ordered Na$_{x}$CoO$_{2}$, for $0.65<x<0.8$. Above 100 K they display similar Curie-Weiss susceptibilities as well as ferromagnetic $q=0$ spin fluctuations in the CoO$_{2}$ planes revealed by $^{23}$Na NMR data. In all phases from $^{59}$Co NMR data we display evidences that the Co disproportionate already above 300 K into non magnetic Co$^{3+}$ and magnetic $\approx $Co$^{3.5+}$ sites on which holes delocalize. This allows us to understand that metallic magnetism is favored for these large Na contents. Below 100 K the phases differentiate, and a magnetic order sets in only for $x\gtrsim 0.75$ at $T_{N}=$22 K. We suggest that the charge order also governs the low $T$ energy scales and transverse couplings.
The magnetic and electronic properties of Ba$_4$Ru$_3$O$_{10}$ were investigated by the ab-initio and model calculations. It is shown that nonmagnetic ground state of the one-third Ru$^{4+}$ ions is not due to the correlation effects. It is rather caused by the charge disproportionation between crystallographically different Ru and the molecular orbital formation in the Ru's trimer.
We present results of studies of charge disproportionation (CD) and spin differentiation in Na$_x$CoO$_2$ using the correlated band theory approach (local-density approximation+Hubbard U:LDA+U). The simultaneous CD and gap opening can be followed through a first order charge disproportionation transition. By comparison with experiments, we propose a value of the Coulomb repulsion strength U($x$) that has significant dependence on the carrier concentration $x$, for which we obtain a phase diagram. The connection between the oxygen height and effects of on-site correlation is also reported.
Charge disproportionation (CD) and spin differentiation in Na$_{1/2}$CoO$_2$ are studied using the correlated band theory approach. The simultaneous CD and gap opening seen previously is followed through a first order charge disproportionation transition 2Co$^{3.5+} \to$ Co$^{3+}$+Co$^{4+}$, whose ionic identities are connected more closely to spin (S=0, S=1/2 respectively) than to real charge. Disproportionation in the Co $a_g$ orbital is compensated by opposing charge rearrangement in other 3d orbitals. At the transition large and opposing discontinuities in the (all-electron) kinetic and po…
The strength and effect of Coulomb correlations in the (superconducting when hydrated) x~1/3 regime of Na(x)CoO(2) have been evaluated using the correlated band theory LDA+U method. Our results, neglecting quantum fluctuations, are: (1) there is a critical $U_{c}$ = 3 eV, above which charge ordering occurs at x=1/3, (2) in this charge-ordered state, antiferromagnetic coupling is favored over ferromagnetic, while below $U_{c}$, ferromagnetism is favored; and (3) carrier conduction behavior should be very asymmetric for dopings away from x=1/3. For x < 1/3, correlated hopping of parallel spin pa…
We have synthesized and characterized different stable phases of sodium cobaltates Na$_{x}$CoO$_{2}$ with sodium content $0.65<x<0.80$. We demonstrate that $^{23}$Na NMR allows to determine the difference in the susceptibility of the phases and reveals the presence of Na order in each phase. $^{59}$Co NMR experiments give clear evidence that Co charge disproportionation is a dominant feature of Na cobaltates. Only a small fraction ($\approx$ 25%) of cobalts are in a non-magnetic Co$^{3+}$ charge state whereas electrons delocalize on the other cobalts. The magnetic and charge properties of the …
The strength and effect of Coulomb correlations in the (superconducting when hydrated) x~1/3 and ``enhanced'' x~2/3 regimes of Na(x)CoO2 are evaluated using the correlated band theory LDA+U method. Our results, neglecting quantum fluctuations, are: (1) allowing only ferromagnetic order, there is a critical U_c = 3 eV, above which charge disproportionation occurs for both x=1/3 and x=2/3, (2) allowing antiferromagnetic order at x=1/3, U_c drops to 1 eV for disproportionation, (3) disproportionation and gap opening occur simultaneously, (4) in a Co(3+)-Co(4+) ordered state, antiferromagnetic cou…
Recently the unusual metallic state with a substantially non-uniform distribution of a charge and mag\-ne\-tic density in CoO$_2$ planes was found experimentally in the Na$_x$CoO$_2$ compound with $x>0.6$. We have investigated an origin of such electron disproportionation in the lamellar sodium cobaltates by calculating the ion states as a function of a strength of the electron correlations in the $d$(Co)-shells within the GGA+U approximation for the system with a realistic crystal structure. It was found that the nonuniformity of spin and charge densities are induced by an ordering of the sod…
To resolve the microscopic origin of magnetism in the Fe2O3/FeTiO3-system, we have performed density functional theory calculations taking into account on-site Coulomb repulsion. By varying systematically the concentration, distribution and charge state of Ti in a hematite host, we compile a phase diagram of the stability with respect to the end members and find a clear preference to form layered arrangements as opposed to solid solutions. The charge mismatch at the interface is accommodated through Ti4+ and a disproportionation in the Fe contact layer into Fe2+, Fe3+, leading to uncompensated…
$^{59}$Co NMR experiments have been performed on single crystals of the layered cobaltate Na$_{x}$CoO$_{2}$ with x=0.77 which is an antiferromagnet with Néel temperature $T_{N}=22$~K. In this metallic phase six Co sites are resolved in the NMR spectra, with distinct quadrupole frequencies $ν_{Q}$, magnetic shifts $K_{ZZ}$ and nuclear spin lattice relaxation rates $% 1/T_{1}$. Contrary to the $x=1/2$ or $x=2/3$ phases the 3D stacking of the Na planes is not perfect for $x=0.77$ but this does not influence markedly the electronic properties. We evidence that the magnetic and charge properties of…
We investigate the impact of electron-lattice coupling on the stability of various magnetic orders in rare-earth nickelates. We use the Hartree-Fock approximation, at zero temperature, to study an effective, two-band model with correlations characterized by a Hubbard $U$ and a Hund's $J$. This is coupled to breathing-mode distortions of the octahedral oxygen cages, described semi-classically, with a Holstein term. We analyze the effect of the various parameters on the resulting phase diagram, in particular on the charge disproportionation and on the magnetic order. We confirm that the coupling…
Ab initio band theory including correlations due to intra-atomic repulsion is applied to study charge disproportionation and charge- and spin-ordering in insulating Na$_{0.5}$CoO$_2$. Various ordering patterns (zigzag and two striped) for four-Co supercells are analyzed before focusing on the observed "out-of-phase stripe" pattern of antiferromagnetic Co$^{4+}$ spins along charge-ordered stripes. This pattern relieves frustration and shows distinct analogies with the cuprate layers: a bipartite lattice of antialigned spins, with axes at 90 degree angles. Substantial distinctions with cuprates …
Nominally pure undoped parent manganite LaMnO_3 exhibits a puzzling behavior inconsistent with a simple picture of an A-type antiferromagnetic insulator (A-AFI) with a cooperative Jahn-Teller ordering. We do assign its anomalous properties to charge transfer instabilities and competition between insulating A-AFI phase and metallic-like dynamically disproportionated phase formally separated by a first-order phase transition at T_{disp}=T_{JT}\approx 750 K. The unconventional high-temperature phase is addressed to be a specific electron-hole Bose liquid (EHBL) rather than a simple "chemically" d…
We report a high-resolution neutron diffraction study of the crystal and magnetic structure of the orbitally-degenerate frustrated metallic magnet AgNiO2. At high temperatures the structure is hexagonal with a single crystallographic Ni site, low-spin Ni3+ with spin-1/2 and two-fold orbital degeneracy, arranged in an antiferromagnetic triangular lattice with frustrated spin and orbital order. A structural transition occurs upon cooling below 365 K to a tripled hexagonal unit cell containing three crystallographically-distinct Ni sites with expanded and contracted NiO6 octahedra, naturally expl…
We report on a study on a representative set of Fe$_{2}$P-based MnFePSi samples by means of $^{55}$Mn NMR in both zero and applied magnetic field. The first-order nature of the magnetic transition is demonstrated by truncated order parameter curves with a large value of the local ordered moment at the Curie point, even at compositions where the transition appears second order from magnetic measurements. No weak ferromagnetic order could be detected at Si-poor compositions showing the kinetic arrest phenomenon, but rather the phase separation of fully ferromagnetic domains from volume fractions…
We analyze the origin of the three dimensional (3D) magnetism observed in nonhydrated Na-rich Na$_x$CoO$_2$ within an itinerant spin picture using a 3D Hubbard model. The origin is identified as the 3D nesting between the inner and outer portions of the Fermi surface, which arise due to the local minimum structure of the $a_{1g}$ band at the $Γ$-A line. The calculated spin wave dispersion strikingly resembles the neutron scattering result. We argue that this 3D magnetism and the spin fluctuations responsible for superconductivity in the hydrated systems share essentially the same origin.
$^{59}$Co NMR spectra in oriented powders of Na$_{0.35}$CoO$_{2}$ and in its hydrated superconducting phase (HSC) Na$_{0.35}$CoO$_{2}$,1.3H$_{2}$O reveal a single electronic Co state with identical $T$ independent NMR shift tensor. These phases differ markedly from Na$_{0.7}$CoO$_{2}$, in which we resolve 3 types of Co sites. The large T variation of their spin susceptibilities $χ^{s}$ and the anisotropy of the orbital susceptibility $χ^{orb}$ allow us to conclude that charge disproportionation occurs, in a non magnetic Co$^{3+}$ and two magnetic sites with about 0.3 and 0.7 holes in the $t_{2…
The effects of the application of a magnetic field on the diagonal stripe spin-glass phase is studied in lightly doped La_{2-x}Sr_xCuO_4 (x=0.014 and 0.024). With increasing magnetic field, the magnetic elastic intensity at the diagonal incommensurate (DIC) positions (1,\pmε,0) decreases as opposed to the increase seen in superconducting samples. This diminution in intensity with increasing magnetic field originates from a spin reorientation transition, which is driven by the antisymmetric exchange term in the spin Hamiltonian. On the other hand, the transition temperature, the incommensurabil…
Epitaxial thin films of undoped LaCoO$_{3}$\@, of electron-doped La$_{0.7}$Ce$_{0.3}$CoO$_{3}$\@, and of hole-doped La$_{0.7}$Sr$_{0.3}$CoO$_{3}$\@ exhibit ferromagnetic order with a transition temperature $T_{\rm{C}}$ $\approx$ 85 K, 22 K, and 240 K, respectively. The spin-state structure for these compounds was studied by soft x-ray magnetic circular dichroism at the Co $L_{2,3}$ and O $K$ edges. It turns out that a higher spin state of the Co$^{3+}$ ions is responsible for the magnetism in LaCoO$_{3}$\@ while for La$_{0.7}$Ce$_{0.3}$CoO$_{3}$ the Co$^{3+}$ ions are in a low-spin state and t…
We employ a combination of density functional theory and dynamical mean-field theory to investigate the electronic structure of the recently synthesized insulator BaCrO$_3$. Our calculations show that Hund's coupling is responsible for strong correlation effects, which are however not sufficient to turn the system insulating. A finite Jahn-Teller distortion lifting the orbital degeneracy is necessary to stabilize an insulating state with orbital ordering and consequent magnetic ordering.
The magnetization rotation transition occurs in the itinerant ferromagnet URhGe when the field about 12T is applied in direction perpendicular to spontaneous magnetization in the plane of the smallest magnetic anisotropy energy.The transition is accompanied by the maximum of resistivity in the normal state and by reentrance of superconductivity at lower temperatures in the field interval between 8 and 13 Tesla [F.Levy et al, Science, to be published (2005)]. We discuss the magnetization orientation transition and the modification of triplet pairing superconducting state coexisting with ferroma…
The cobaltates have demonstrated a wide variety complex behavior. The Na rich region of the phase diagram displays various degrees of anomalous behavior, such as Curie-Weiss behavior near a band insulator\cite{Foo:2004}, charge disproportionation\cite{Mukhamedshin:2005}, and non-Fermi-liquid behavior in the resistivity\cite{Foo:2004}. Alternatively, the Na poor region of the phase diagram appears to be a Fermi-liquid. The magnetic susceptibility displays Pauli behavior, the resistivity is roughly quadratic at low temperatures\cite{Foo:2004}, and the system appears to be homogeneous\cite{Mukham…
We study the interplay between correlation, itinerant ferromagnetism and local moment formation on the electron doped triangular lattice of sodium cobaltates Na$_x$CoO$_2$. We find that strong correlation renormalizes the Stoner criterion and stabilizes the paramagnetic state for $x<x_c\simeq0.67$. For $x>x_c$, ferromagnetic (FM) order emerges. The enhanced Na dopant potential fluctuations play a crucial role in the sodium rich phases and lead to an inhomogeneous FM state, exhibiting nonmagnetic Co$^{3+}$ patches, antiferromagnetic (AF) correlated regions, and FM clusters with AF domains. Hole…
We have prepared a series of polycrystalline samples La$_{0.5}$Sr$_{0.5}$CoO$_{3-δ}$} with $0 < δ\le 0.21$ and characterized their oxygen content, crystal structure, and magnetic properties. While the fully oxygenated samples are good ferromagnets, samples with larger $δ$ values display increasingly broad magnetic transitions. The saturation magnetization at 5 K falls rapidly as $δ$ increases. First principles electronic structure calculations provide insights into the magnetic behavior of the fully oxygenated compound, and the manner in which ferromagnetic ordering is affected by increasing o…
Electrical control of magnetism is a long-standing goal in physics and technology, recently developed electrolyte gating techniques providing a promising route to realization. Validating a recent theoretical prediction, here we demonstrate large enhancement of electrostatic modulation of ferromagnetic order in ion-gel-gated ultrathin La$_{0.5}$Sr$_{0.5}$CoO$_{3-δ}$ by thickness-tuning to the brink of a magnetic percolation transition. Application of only 3-4 V then drives a transition from a short-range-ordered insulator to a robust long-range ferromagnetic metal, realizing giant electrostatic…
We report on zero-field muon spin relaxation studies of cerium based heavy-fermion materials CeRh_{1-x}Ir_xIn_5. In the superconducting x=0.75 and 1 compositions muon spin relaxation functions were found to be temperature independent across T_c; no evidence for the presence of electronic magnetic moments was observed. The x=0.5 material is antiferromagnetic below T_N=3.75 K and superconducting below T_c=0.8 K. Muon spin realxation spectra show the gradual onset of damped coherent oscillations characteristic of magnetic order below T_N. At 1.65 K the total oscillating amplitude accounts for at …
We report neutron scattering measurements on single crystals of BaFe$_{1.92}$Co$_{0.08}$As$_2$. The magnetic Bragg peak intensity is reduced by 6 % upon cooling through T$_C$. The spin dynamics exhibit a gap of 8 meV with anisotropic three-dimensional (3d) interactions. Below T$_C$ additional intensity appears at an energy of $\sim$4.5(0.5) meV similar to previous observations of a spin resonance in other Fe-based superconductors. No further gapping of the spin excitations is observed below T$_C$ for energies down to 2 meV. These observations suggest the redistribution of spectral weight from …
The recent discovery of pressure induced superconductivity in the binary helimagnet CrAs has attracted much attention. How superconductivity emerges from the magnetic state and what is the mechanism of the superconducting pairing are two important issues which need to be resolved. In the present work, the suppression of magnetism and the occurrence of superconductivity in CrAs as a function of pressure ($p$) were studied by means of muon spin rotation. The magnetism remains bulk up to $p\simeq3.5$~kbar while its volume fraction gradually decreases with increasing pressure until it vanishes at …
We review the normal and superconducting state properties of the unconventional triplet superconductor Sr$_2$RuO$_4$ with an emphasis on the analysis of the magnetic susceptibility and the role played by strong electronic correlations. In particular, we show that the magnetic activity arises from the itinerant electrons in the Ru $d$-orbitals and a strong magnetic anisotropy occurs ($χ^{+-} < χ^{zz}$) due to spin-orbit coupling. The latter results mainly from different values of the $g$-factor for the transverse and longitudinal components of the spin susceptibility (i.e. the matrix elements d…
We have compared by $^{23}$Na NMR and magnetic susceptibility the magnetic properties of oriented powder samples of Na$_{x}$CoO$_{2}$ compounds. The NMR spectra are found identical for various samples with nominal $0.50\leq x\leq 0.70,$ which establishes that the dominant phase has a single composition $x\approx 0.70$. Three Na sites are identified from their single valued quadrupole effects and magnetic shifts which implies a very definite order of the Na$^{+}$ ions and of the Co charges in the CoO$_{2}$ planes. The local susceptibility of the magnetic cobalt sites displays a large enhancemen…
The title compound Ba3RuTi2O9 crystallizes with a hexagonal unit cell. It contains layers of edge shared triangular network of Ru4+ (S=1) ions. Magnetic susceptibility chi(T) and heat capacity data show no long range magnetic ordering down to 1.8K. A Curie-Weiss (CW) fitting of chi(T) yields a large antiferromagnetic CW temperature theta_CW=-166K. However, in low field, a splitting of zero field cooled (ZFC) and field cooled (FC) chi(T) is observed below ~30K. Our measurements suggest that Ba3RuTi2O9 is a highly frustrated system but only a small fraction of the spins in this system undergo a …
$\rm CePt_3Si$ is a novel ternary compound exhibiting antiferromagnetic order at $T_N \approx 2.2$ K and superconductivity (SC) at $T_c \approx 0.75$ K. Large values of $H_{c2}' \approx -8.5$ T/K and $H_{c2}(0) \approx 5$ T indicate Cooper pairs formed out of heavy quasiparticles. The mass enhancement originates from Kondo interaction with a characteristic temperature $T_K \approx 8$ K. NMR and $μ$SR measurements evidence coexistence of SC and long range magnetic order on a microscopic scale. Moreover, $\rm CePt_3Si$ is the first heavy fermion SC without an inversion symmetry. This gives rise …
A C14 Nb0.975Fe2.025 Laves phase compound was investigated aimed at determining the H-T magnetic phase diagram. Magnetization, M, and AC magnetic susceptibility measurements were performed. Concerning the former field-cooled and zero-field-cooled M-curves were recorded in the temperature range of 2-200K and in applied magnetic field, H, up to 1000 Oe, isothermal M(H) curves at 2 K, 5 K, 50 K, 80 K and 110 K as well as hysteresis loops at several temperatures over the field range of -10 to +10kOe. Regarding the AC susceptibility, both real and imaginary components were registered as a function …
We systematically investigate the magnetic properties and local structure of Ba2YIrO6 to demonstrate that Y and Ir lattice defects in the form of antiphase boundary or clusters of antisite disorder affect the magnetism observed in this $d^4$ compound. We compare the magnetic properties and atomic imaging of (1) a slow cooled crystal, (2) a crystal quenched from 900\degree C after growth, and (3) a crystal grown using a faster cooling rate than the slow cooled one. Atomic imaging by scanning transmission electron microscopy (STEM) shows that quenching from 900oC introduces antiphase boundary to…
We prove the direct link between low temperature magnetism and high temperature sodium ordering in NaxCoO2 using the example of a heretofore unreported magnetic transition at 8 K which involves a weak ferromagnetic moment. The 8 K feature is characterized in detail and its dependence on a diffusive sodium rearrangement around 200 K is demonstrated. Applying muons as local probes this process is shown to result in a reversible phase separation into distinct magnetic phases that can be controlled by specific cooling protocols. Thus the impact of ordered sodium Coulomb potential on the CoO2 physi…
We review examples of muon-spin relaxation measurements on molecule-based magnetic coordination polymers, classified by their magnetic dimensionality. These include the one-dimensional s=1/2 spin chain Cu(pyz)(NO3)2 and the two-dimensional s=1/2 layered material [Cu(HF2)(pyz)2]BF4. We also describe some of the more exotic ground states that may become accessible in the future given the ability to tune the interaction strengths of our materials through crystal engineering.
C14 Nb(Fe89.4Al10.6)2 Laves phase intermetallic compound was investigated by DC magnetization (M) measurements performed in the temperature (T) interval of 20 to 175 K,under an applied magnetic field (H) ranging between 50 and 1250 Oe. Magnetization curves were recorded in the field-cooled (FC) and in the zero-field-cooled (ZFC) modes. They clearly showed an irreversible character that vanished at H=1250 Oe. Both magnetization curves exhibited well-defined peaks around T_N =72.3 K whose positions were H-independent, so they were identified as the compound's Néel temperature. The existence of i…
Specific heat of the layered NaxCoO2 (x=0.65, 0.70 and 0.75) oxides has been measured in the temperature range of 3-360 K and magnetic field of 0 and 9 T. The analysis of data, assuming the combined effect of inter-layer superexchange and the phase separation into mesoscopic magnetic domains with localized spins embedded in a matrix with itinerant electronic character, suggests that the dominant contribution to the specific heat in the region of short-range ordering is mediated by quasi-2D antiferromagnetic clusters, perpendicular to the CoO2 layers.
A macroscopic single crystal of $γ_{\rm II}$-Li\(_2\)FeSiO\(_4\) has been grown by means of the high-pressure optical floating-zone technique. Static magnetic susceptibility $χ$ implies that the tetrahedrally-coordinated Fe$^{2+}$ ions are in the high-spin, $S=2$, state. While a sharp decrease in $χ$ implies long-range antiferromagnetic order below \tn\ = 17.0(5)~K, the presence of a broad maximum at $T_{\rm m} = 28$~K suggests quasi-low-dimensional magnetism. Applying magnetic fields along the easy magnetic $a$-axis yields additional contributions to the susceptibility $\partial M/\partial B$…
In recent years, the optical control of exchange interactions has emerged as an exciting new direction in the study of the ultrafast optical control of magnetic order. Here we review recent theoretical works on antiferromagnetic systems, devoted to i) simulating the ultrafast control of exchange interactions, ii) modeling the strongly nonequilibrium response of the magnetic order and iii) the relation with relevant experimental works developed in parallel. In addition to the excitation of spin precession, we discuss examples of rapid cooling and the control of ultrafast coherent longitudinal s…
The magnetic properties and structure of LixCoO2 for x between 0.5 and 1.0 are reported. Co4+ is found to be high-spin in LixCoO2 for x between 0.94 and 1.0 and low-spin for x between 0.50 and 0.78. Weak antiferromagnetic coupling is observed, increasing in strength as more Co4+ is introduced. At an x value of about 0.65, the temperature-independent contribution to the magnetic susceptibility and the electronic contribution to the specific heat are largest. Neutron diffraction analysis reveals that the lithium oxide layer expands perpendicular to the basal plane and the Li ions displace from t…
We propose an explanation for the experiment by Schemm et al., Phys. Rev. B 91, 140506 (2015) where the polar Kerr effect (PKE), indicating time-reversal symmetry (TRS) breaking, was observed in the hidden-order (HO) phase of URu2Si2. The PKE signal on warmup was seen only if a training magnetic field was present on cool-down. Using a Ginzburg-Landau model for a complex order parameter, we show that the system can have a metastable ferromagnetic state producing the PKE, even if the HO ground state respects TRS. We predict that a strong reversed magnetic field should reset the PKE to zero.
$^{13}$C NMR observation of a nonmagnetic charge-ordered state in the organic conductor $κ$-(ET)$_{2}$Hg(SCN)$_{2}$Cl
University of Tokyo（东京大学）；The Institute for Solid State Physics, University of Tokyo（东京大学固体物理研究所）；Institute of Problems of Chemical Physics RAS（俄罗斯科学院化学物理问题研究所）；The Institute for Quantum Matter and the Department of Physics and Astronomy, The Johns Hopkins University（约翰斯·霍普金斯大学量子物质研究所及物理与天文学系）；Max Planck Institute for Solid State Research（马克斯·普朗克固体研究所）；University of Stuttgart（斯图加特大学）；Department of Advanced Materials Science, University of Tokyo（东京大学先进材料科学系）
We performed muon spin rotation/relaxation measurements to investigate the magnetic behavior of $T^{\prime}$-type Eu$_2$CuO$_4$ (ECO), which is the parent compound of electron-doped cuprate superconductors, and the effects of oxygen-reduction annealing on its magnetism. In as-sintered (AS) ECO, we clarified the development of magnetic correlations upon cooling below $T_\mathrm{N1}$ (= 265 K) as well as the coexistence of a dominant fluctuating spin state and partially ordered spin state in the temperature range between $\sim$150 K and $T_\mathrm{N1}$. Upon further cooling, uniform long-range m…
The magnetic phase diagram in the H-T coordinates has been determined for σ-Fe68V32 from the ZFC/FC magnetization measurements. The re-entrant character of magnetism, going from paramagnetic through ferromagnetic to spin-glass (SG) states, has been evidenced. The SG phase is magnetically heterogeneous, because two sub phases can be identified i.e. with the strong (SG-SI) and the weak (SG-WI) irreversibility. The ireversibility, T_irr and the crossover, T_cros, temperatures were quantitatively analysed using the mean-field theory and ϕ_irr=1.6(2) and ϕ_cros=0.91(9) values were obtained. A quali…
We compute the electronic structure, spin and charge state of Fe ions, and structural phase stability of paramagnetic CaFeO$_3$ under pressure using a fully self-consistent in charge density DFT+dynamical mean-field theory method. We show that at ambient pressure CaFeO$_3$ is a negative charge-transfer insulator characterized by strong localization of the Fe $3d$ electrons. It crystallizes in the monoclinic $P2_1/n$ crystal structure with a cooperative breathing mode distortion of the lattice. While the Fe $3d$ Wannier occupations and local moments are consistent with robust charge disproporti…
Quantum many body phases, in competition or coexistence has always been a fascinating area of research in condensed matter physics. One of the most widely investigated scenario of phase competition is that between superconductivity and magnetism, which in spite of several decades of research continues to bring up new surprises till date. While superconductivity and magnetism are naively considered to be antagonists, there are several circumstances where these many body phases can be found to be cooperating, coexisting and even promoting each other. The results of such cooperative behavior are …
The iron arsenide Eu3Fe2O5Fe2As2 was synthesized at 1173-1373 K in a resistance furnace and characterized by X-ray powder diffraction with Rietveld analysis: Sr3Fe2O5Cu2S2-type, I4/mmm, a = 406.40(1) pm, c = 2646.9(1) pm. Layers of edge-sharing FeAs4/4 tetrahedra are separated by perovskite-like oxide blocks. No structural transition occurs in the temperature range from 10 to 300 K. Magnetic measurements have revealed Curie-Weiss behavior with an effective magnetic moment of 7.79 muB per europium atom in agreement with the theoretical value of 7.94 muB for Eu2+. A drop in the magnetic suscepti…
We study magnetic, transport and thermodynamic properties of the half-filled two-dimensional ($2D$) Hubbard model with layered distributed repulsive interactions using unbiased finite temperature quantum Monte Carlo simulations. Antiferromagnetic long-ranged correlations at $T=0$ are confirmed by means of the magnetic structure factor and the onset of short-ranged ones is at a minimum temperature which can be obtained by peaks in susceptibility and specific heat following an RPA prediction. We also show that transport is affected in the large interaction limit and is enhanced in the non-repuls…
(TMTTF)2AsF6 undergoes two phase transitions upon cooling from 300 K. At Tco=103 K a charge-ordering (CO) occurs, and at Tsp(B=9 T)=11 K the material undergoes a spin-Peierls (SP) transition. Within the intermediate, CO phase, the charge disproportionation ratio is found to be at least 3:1 from carbon-13 NMR 1/T1 measurements on spin-labeled samples. Above Tsp, up to about 3Tsp, 1/T1 is independent of temperature, indicative of low-dimensional magnetic correlations. With the application of about 0.15 GPa pressure, Tsp increases substantially, while Tco is rapidly suppressed, demonstrating that…
α-SrCr2O4 has a triangular planar lattice of d3 Cr3+ made from edge sharing CrO6 octahedra; the plane shows a very small orthorhombic distortion from hexagonal symmetry. With a Weiss temperature of -596 K and a three-dimensional magnetic ordering temperature of 43 K, the magnetic system is quasi two-dimensional and frustrated. Neutron powder diffraction shows that the ordered state is an incommensurate helical magnet, with an in-plane propagation vector of k = (0,0.3217(8),0). Temperature dependent synchrotron powder diffraction characterization of the structure shows an increase in the inter-…
The evolution of the magnetic ordering temperature of the 4d3 perovskites RTcO3 (R=Ca,Sr,Ba) and its relation with its electronic and structural properties has been studied by means of hybrid density functional theory and Monte Carlo simulations. When compared to the most widely studied 3d perovskites the large spatial extent of the 4d shells and their relatively strong hybridization with oxygen weaken the tendency to form Jahn-Teller like orbital ordering. This strengthens the superexchange interaction. The resulting insulating G-type antiferromagnetic ground state is characterized by large s…
When superconductivity couples with noncollinear spin textures, rich physics arises; for instance, singlet Cooper pairs can be converted to triplet pairs, and topological superconductors can be realized. For their applications, the controllability of noncollinear magnetism is a crucial issue. Here, we propose that a supercurrent can induce and control noncollinear magnetic orders in a correlated metal on top of a singlet superconductor. We show that the magnetic instability in the correlated metal is enhanced by the proximity effect of supercurrents, which leads to phase transitions from a par…
Composite multiferroics are materials exhibiting the interplay of ferroelectricity, magnetism, and strong electron correlations. Typical example --- magnetic nano grains embedded in a ferroelectric matrix. Coupling of ferroelectric and ferromagnetic degrees of freedom in these materials is due to the influence of ferroelectric matrix on the exchange coupling constant via screening of the intragrain and intergrain Coulomb interaction. Cooling typical magnetic materials the ordered state appears at lower temperatures than the disordered state. We show that in composite multiferroics the ordered …
Sigma-phase intermetallic compound of Fe54Cr46 was investigated using DC and AC magnetic susceptibility techniques. A clear-cut evidence was found that the sample orders magnetically at Tc=23.5 K and its ground magnetic state is constituted by a spin glass. The temperature at which the zero-field cooled magnetization has its maximum decreases with an external magnetic field in line with the Gabay-Toulouse prediction. The temperature at which the AC magnetic susceptibility has its maximum does not depend on frequency which, in the light of the mean-field theory, testifies to very long magnetic …
A detailed study of the low-temperature magnetic state and the relaxation in the phase-separated colossal magnetoresistance Nd2/3Ca1/3MnO3 perovskite has been carried out. Clear experimental evidence of the cluster-glass magnetic behavior of this compound has been revealed. Well defined maxima in the in-phase linear ac susceptibility $χ^{/}(T)$ were observed, indicative of the magnetic glass transition at $T_{g}$ = 60 K. Strongly divergent zero-field-cooled and field-cooled static magnetizations and frequency dependent ac susceptibility are evident of the glassy-like magnetic state of the comp…
Two-dimensional (2D) metal-organic frameworks (MOFs) in a kagome lattice can exhibit strong electron-electron interactions, which can lead to tunable quantum phases including many exotic magnetic phases. While technological developments of 2D MOFs typically take advantage of substrates for growth, support, and electrical contacts, investigations often ignore substrates and their dramatic influence on electronic properties of MOFs. Here, we show how substrates alter the correlated magnetic phases in kagome MOFs using systematic density functional theory and mean-field Hubbard calculations. We d…
We report an x-ray emission spectroscopy (XES) study of the local fluctuating magnetic moment ($μ_{bare}$) in $\mathrm{NaFe_{1-x}Co_{x}As}$ and $\mathrm{NaFe_{1-x}Cu_{x}As}$. In NaFeAs, the reduced height of the As ions induces a local magnetic moment higher than $\mathrm{Ba_2As_2}$, despite lower T$_N$ and ordered magnetic moment. As NaFeAs is doped with Co $μ_{bare}$ is slightly reduced, whereas Cu doping leaves it unaffected, indicating a different doping mechanism: based on electron counting for Co whereas impurity scattering dominates in the case of Cu. Finally, we observe an increase of …
We present key issues of related phenomenons of the Ferroelectricity and the Charge Disproportionation in organic metals. In (TMTTF_2X the dielectric susceptibility demonstrates clear cases of the ferroelectric and anti-ferroelectric phase transitions. Both the susceptibility and the conductivity prove independence and occasional coexistence of "structurless" ferroelectric transitions and usual "anionic" ones. Their sequence gives access to physics of three types of solitons emerging upon cooling via several steps of symmetry breaking. The theory invokes a concept of the Combined Mott-Hubbard …
