We report Raman scattering experiments on the strongly correlated electron system NaxCoO2 with x= 0.71 and ordered Na vacancies. In this doping regime, NaxCoO2 exhibits a large and unusual thermopower and becomes superconducting upon hydration. Our Raman scattering data reveal pronounced low energy fluctuations that diverge in intensity at low temperatures. Related to these fluctuations is a drastic decrease of an electronic scattering rate from 50 to 3 cm-1. This observation is quite different from the behavior of Na disordered samples that have a larger and temperature independent scattering rate. Simultaneously with the evolution of the scattering rate, phonon anomalies point to an increasing out-of-plane coherence of the lattice with decreasing temperature. These observations may indicate the condensation of spin polarons into an unusual, highly dynamic ground state.
Herein, we report the magneto-transport and exchange bias effect in a "314 - type" oxygen - vacancy ordered material with composition SrCo$_{0.85}$Fe$_{0.15}$O$_{2.62}$. This material exhibits a ferrimagnetic transition above room temperature, at 315 K. The negative magnetoresistance starts to appear from room temperature (-1.3 $\%$ at 295 K in 70 kOe) and reaches a sizable value of 58 $\%$ at 4 K in 70 kOe. Large exchange bias effect is observed below 315 K when the sample is cooled in the presence of a magnetic field. The coexistence of nearly compensated and ferrimagnetic regions in the lay…
We report the structural, magnetic, exchange bias and magnetotransport effect in Sr$_{4}$Fe$_{3}$CoO$_{11}$. The material crystallizes in the orthorhombic $\textit{Cmmm}$ space group. It shows antiferromagnetic (G-type) transition (T$_{N}$ = 255 K) along with interesting temperature induced magnetization reversal (T$_{Comp.}$= 47 K measured at 100 Oe). The magnetic reversal can be elucidated considering the increased magnetocrystalline anisotropy with Co substitution. Magnetoresistance measurements shows an interesting crossover from negative to positive side at $\sim$ 100 K. The negative magn…
We have synthesized A-site ordered (AO)- and A-site disordered (AD)-Y1/4Sr3/4CoO3-delta (YSCO) with various oxygen deficiency delta, and have made a comparative study of the structural and physical properties. We have found that A-site (Y/Sr) ordering produces the unconventional oxygen-vacancy ordered (OO) structure, and that the magnetic and transport properties of both AO- and AD-YSCO strongly depend on the oxygen-vacancy (or excess oxygen) ordering pattern. AO-YSCO with a stoichiometric delta of 0.5 has the unconventional OO structure reflecting Y/Sr ordering pattern. With decreasing delta …
We investigate the electronic structure of the ternary iron selenide K$_{y}$% Fe$_{1.6}$Se$_{2}$ by considering the spatial symmetry of the $\sqrt{5}% \times \sqrt{5}$ vacancy ordered structure. Based on three orbitals of $% t_{2g}$, which are believed to play major physics in iron-based superconductors, an effective two-dimensional tight binding Hamiltonian is constructed with the vacancy ordered structure being explicitly included. It is shown that the constructed band model, when combined with generalized Hubbard interactions, yields a spin susceptibility which exhibits both the block-check…
We unveil the novel physical origin of the insulating block checkerboard antiferromagnetism in vacancy-ordered K2Fe4Se5. Our first-principles electronic structure analysis reveals its incompatibility with a simple Fermi-surface nesting or Mott insulator scenario, and suggests the picture of coexisting itinerant and localized electronic states. Consistently, we demonstrate that it can be unified with the metallic collinear or bicollinear antiferromagnetism of the vacancy-free parent compounds LaOFeAs, BaFe2As2, or FeTe in the spin-fermion model. These results indicate that the blocking effects …
Phase diagram of Na$_x$CoO$_2$ (x $\gtrsim$ 0.71) has been reinvestigated using electrochemically fine tuned single crystals. Both phase separation and staging phenomena as a result of sodium multi-vacancy cluster ordering have been found. Phase separation phenomenon is observed in the narrow ranges of 0.76 $\lesssim$ x $\lesssim$ 0.82 and 0.83 $\lesssim$ x $\lesssim$ 0.86. While x = 0.820 shows A-type antiferromagnetic (A-AF) ordering below 22K, x = 0.833 is confirmed to have a magnetic ground state of A-AF ordering below $\sim$8K and is only reachable through slow cooling. In addition, x = 0…
Based on an effective 12-orbital tight-binding model, we examine the superconducting states induced by the antiferromagnetic fluctuations for iron-vacancy-ordered A$_{y}$Fe$_{2-x}$Se$_{2}$. It is shown that due to the broken reflection symmetry induced by the iron vacancies, new superconducting states with $C_{4h}$ symmetry emerge. In particular, we show that in the $C_{4h}$ symmetry, symmetric axes of the pairing momenta do not need to coincide with axes of the unit cell. As a result, in addition to the magnitude of the pairing gap, the relative orientation of the pairing wave function to the…
The electronic structure of the vacancy-ordered K$_{0.5}$Fe$_{1.75}$Se$_2$ iron-selenide compound (278 phase) is studied using the first-principles density functional method. The ground state of the 278 phase is stripe-like antiferromagnetic, and its bare electron susceptibility shows a large peak around $(π, π)$ in the folded Brillouin zone. Near Fermi level, the density of states are dominated by the Fe-3d orbitals, and both electron-like and hole-like Fermi surfaces appear in the Brillouin zone. Unfolded band structure shows limited similarities to a hole doped 122 phase. With 0.1e electron…
Various Fe-vacancy orders have been reported in tetragonal Fe1-xSe single crystals and nanowires/nanosheets, which are similar to those found in alkali metal intercalated A1-xFe2-ySe2 superconductors. Here we report the in-situ angle-resolved photoemission spectroscopy study of Fe-vacancy disordered and ordered phases in FeSe multi-layer thin films grown by molecular beam epitaxy. Low temperature annealed FeSe films are identified to be Fe-vacancy disordered phase and electron doped. Further long-time low temperature anneal can change the Fe-vacancy disordered phase to ordered phase, which is …
Temperature and Pressure Dependent Vibrational Properties of Pristine and Doped Vacancy-Ordered Double Perovskite
National Centre for High Pressure Studies, Department of Physical Sciences, Indian Institute of Science Education and Research Kolkata（印度科学教育研究所加尔各答分校物理科学系高压研究中心）；Indian Institute of Science Education and Research (IISER) Kolkata（印度科学教育研究所加尔各答分校）；Department of Chemical Sciences, and Centre for Advanced Functional Materials, Indian Institute of Science Education and Research (IISER) Kolkata（印度科学教育研究所加尔各答分校化学科学系及先进功能材料中心）
Small Drude weight $D$ together with small specific heat coefficient $γ$ observed in the ferromagnetic phase of R$_{1-x}$A$_x$MnO$_3$ (R=La, Pr, Nd, Sm; A=Ca, Sr, Ba) are analyzed in terms of a proximity effect of the Mott insulator. The scaling theory for the metal-insulator transition with the critical enhancement of orbital correlations toward the staggered ordering of two $e_g$ orbitals such as $3x^2-r^2$ and $3y^2-r^2$ symmetries may lead to the critical exponents of $D \propto δ^{u}$ and $γ\propto δ^v$ with $u=3/2$ and $v=0$. The result agrees with the experimental indications.
The relationship between vacancy ordering and magnetism in TlFe1.6Se2 has been investigated via single crystal neutron diffraction, nuclear forward scattering, and transmission electron microscopy. The examination of chemically and structurally homogenous crystals allows the true ground state to be revealed, which is characterized by Fe moments lying in the ab-plane below 100K. This is in sharp contrast to crystals containing regions of order and disorder, where a competition between c-axis and ab-plane orientations of the moments is observed. The properties of partially-disordered TlFe1.6Se2 …
The microscopic details of the suppression of antiferromagnetic order in the Kondo-lattice series Ce$_{1-x}$La$_{x}$Cu$_{2}$Ge$_{2}$ due to nonmagnetic dilution by La are revealed through neutron diffraction results for $x=0.20$, $0.40$, $0.75$, and $0.85$. Magnetic Bragg peaks are found for $0.20\le x\le0.75$, and both the Néel temperature, $T_{\textrm{N}}$, and the ordered magnetic moment per Ce, $μ$, linearly decrease with increasing $x$. The reduction in $μ$ points to strong hybridization of the increasingly diluted Ce $4f$ electrons, and we find a remarkable quadratic dependence of $μ$ on…
With single crystal X-ray diffraction studies, we compare the structures of three sample showing optimal superconductivity, K0.774(4)Fe1.613(2)Se2, K0.738(6)Fe1.631(3)Se2 and Cs0.748(2)Fe1.626(1)Se2. All have an almost identical ordered vacancy structure with a ({\sqrt}5 x {\sqrt}5 x 1) super cell. The tetragonal unit cell, space group I4/m, possesses lattice parameters at 250K of a = b = 8.729(2) Å and c = 14.120(3) Å, a = b = 8.7186(12) Å and c = 14.0853(19) Å and at 295 K, a = b = 8.8617(16) Å and c = 15.304(3) Å for the three crystals, respectively. The structure contains two iron sites; o…
Breakdown of $J_{eff}$ = 0 and $J_{eff}$ = 3/2 states and existence of large magnetic anisotropy energy in vacancy ordered 5$d$ antifluorites: K$_2$ReCl$_6$, K$_2$OsCl$_6$, and K$_2$IrCl$_6$
Na$_2$Ir$^\text{IV}$Cl$_6$: The Missing Member of the Perfectly Cubic Vacancy Ordered $A_2$IrCl$_6$ Family, Another Potential $J_{eff}$ = $\frac{1}{2}$ Ground State Candidate
Indian Association for the Cultivation of Science（印度科学文化研究所）；Deutsches Elektronen–Synchrotron DESY（德国电子同步辐射中心）；Christian-Albrechts-Universität zu Kiel（基尔大学）
Nitrogen-vacancy center in diamond is a solid state defect qubit with favorable coherence time up to room temperature which could be harnessed in several quantum enhanced sensor and quantum communication applications, and has a potential in quantum simulation and computing. The quantum control largely depends on the intricate details about the electronic structure and states of the nitrogen-vacancy center, radiative and non-radiative rates between these states and the coupling of these states to external spins, electrical, magnetic and strain fields and temperature. In this review paper it is …
We have performed Raman-scattering measurements on a high-quality single crystal of the recently discovered Fe-based superconductor K$_{0.8}$Fe$_{1.6}$Se$_2$ ($T_c$ = 32 K). At least thirteen phonon modes were observed in the wave number range 10$-$300 cm$^{-1}$. The spectra possess a four-fold symmetry indicative of bulk vacancy order in the Fe-deficient planes. We perform a vibration analysis based on first-principles calculations, which both confirms the ordered structure and allows a complete mode assignment. We observe an anomaly at $T_c$ in the 180 cm$^{-1}$ $A_g$ mode, which indicates a…
The high temperature ferromagnetism in Sr3YCo4O10+delta perovskite, whose origin has been the subject of a considerable debate, has been studied by neutron powder diffraction and synchrotron X-ray diffraction measurements. Oxygen vacancy ordering creates a complex pattern of zigzag stripes in the oxygen-deficient CoO4+delta layers, where the Co ions are found in three distinct coordinations. The symmetry of this unprecedented structural modulation, in conjunction with the existence of different Co spin states, provide a straightforward explanation for the appearance of ferrimagnetism. A model …
