arXiv subjects

Athena S. Sefat

Publications and source records attributed to Athena S. Sefat.

At least 55 records · Page 3Linked to original sources

arXiv2015

Superconducting and Structural Features of Tl-1223

This study provides an account of the bulk preparation of TlBa2Ca2Cu3O9-δ (Tl-1223) superconductor at ambient pressure, and the Tc features under thermal-annealing conditions. The as-prepared Tl-1223 (Tc =106 K) presents a significantly higher Tc = 125 K after annealing the polycrystalline material in either flowing Ar+4% H2, or N2 gases. In order to understand the fundamental reasons for a particular Tc, we refined the average bulk structures using powder X-ray diffraction data. Although Ar+4%H2 annealed Tl-1223 shows an increased c lattice parameter, it is approximately unchanged upon N2-anneal. Due to such indeterminate conclusions on the average structural changes, local structures were investigated at using aberration-corrected scanning-transmission electron microscopy technique. Similar compositional changes in the atomic arrangements of both annealed-samples of Tl-1223 were detected in which the plane containing Ca atomic layer gives a non-uniform contrast, due to substitution of some heavier Tl. In this report, extensive bulk properties are summarized through temperature-dependent resistivity, and shielding and Meissner fractions of magnetic susceptibility results; the bulk and local structures are investigated to correlate to properties.

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arXiv2015

Tetragonal and collapsed-tetragonal phases of CaFe2As2 -- a view from angle-resolved photoemission and dynamical mean field theory

We present a study of the tetragonal to collapsed-tetragonal transition of CaFe2As2 using angle-resolved photoemission experiments and dynamical mean field theory-based electronic structure calculations. We observe that the collapsed-tetragonal phase exhibits reduced correlations and a higher coherence temperature due to the stronger Fe-As hybridization. Furthermore, a comparison of measured photoemission spectra and theoretical spectral functions shows that momentum-dependent corrections to the density functional band structure are essential for the description of low-energy quasiparticle dispersions. We introduce those using the recently proposed combined "Screened Exchange + Dynamical Mean Field Theory" scheme.

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arXiv2015

Direct spectroscopic evidence for completely filled Cu $3d$ shell in BaCu$_2$As$_2$ and $α$-BaCu$_2$Sb$_2$

We use angle-resolved photoemission spectroscopy to extract the band dispersion and the Fermi surface of BaCu$_2$As$_2$ and $α$-BaCu$_2$Sb$_2$. While the Cu $3d$ bands in both materials are located around 3.5 eV below the Fermi level, the low-energy photoemission intensity mainly comes from As $4p$ states, suggesting a completely filled Cu $3d$ shell. The splitting of the As $3d$ core levels and the lack of pronounced three-dimensionality in the measured band structure of BaCu$_2$As$_2$ indicate a surface state likely induced by the cleavage of this material in the collapsed tetragonal phase, which is consistent with our observation of a Cu$^{+1}$ oxydation state. However, the observation of Cu states at similar energy in $α$-BaCu$_2$Sb$_2$ without the pnictide-pnictide interlayer bonding characteristic of the collapsed tetragonal phase suggests that the short interlayer distance in BaCu$_2$As$_2$ follows from the stability of the Cu$^{+1}$ rather than the other way around. Our results confirm the prediction that BaCu$_2$As$_2$ is an $sp$ metal with weak electronic correlations.

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arXiv2014

Optimization of a Non-arsenic Iron-based Superconductor for Wire Fabrication

We report on the optimization of synthesis of iron-selenide (non-arsenic) superconducting powders that are based on '122' composition, with optimal Tc = 38 K and Jc = 10^5 A/cm2 (4 K). We also report on the wire proof-of concept for these materials, by producing ~ 40 ft of wire that produce Ic. The 122 selenides are more difficult to synthesize and have more complex crystal structures compared to '11' selenides (FeSe and FeSe1-xTex), but they do offer higher Tc and might provoke a natural extension for 11 work.

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arXiv2014

On the origin of the electronic anisotropy in iron pnicitde superconductors

We use polarization-resolved Raman spectroscopy to study the anisotropy of the electronic characteristics of the iron-pnictide parent compounds $A$Fe$_{2}$As$_{2}$ ($A$~=~Eu, Sr). We demonstrate that above the structural phase transition at Ts the dynamical anisotropic properties of the 122 compounds are governed by the emergence of $xy$-symmetry critical collective mode foretelling a condensation into a state with spontaneously broken four-fold symmetry at a temperature $T^{*}$. However, the mode's critical slowing down is intervened by a structural transition at Ts, about 80~K above $T^{*}$, resulting in an anisotropic density wave state.

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arXiv2014

Orbital occupancy and charge doping in iron-based superconductors

Iron-based superconductors (FBS) comprise several families of compounds having the same atomic building blocks for superconductivity, but large discrepancies among their physical properties. A longstanding goal in the field has been to decipher the key underlying factors controlling TC and the various doping mechanisms. In FBS materials this is complicated immensely by the different crystal and magnetic structures exhibited by the different families. In this paper, using aberration-corrected scanning transmission electron microscopy (STEM) coupled with electron energy loss spectroscopy (EELS), we observe a universal behavior in the hole concentration and magnetic moment across different families. All the parent materials have the same total number of electrons in the Fe 3d bands; however, the local Fe magnetic moment varies due to different orbital occupancy. Although the common understanding has been that both long-range and local magnetic moments decrease with doping, we find that, near the onset of superconductivity, the local magnetic moment increases and shows a dome-like maximum near optimal doping, where no ordered magnetic moment is present. In addition, we address a longstanding debate concerning how Co substitutions induces superconductivity in the 122 arsenide family, showing that the 3d band filling increases a function of doping. These new microscopic insights into the properties of FBS demonstrate the importance of spin fluctuations for the superconducting state, reveal changes in orbital occupancy among different families of FBS, and confirm charge doping as one of the mechanisms responsible for superconductivity in 122 arsenides.

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arXiv2014

Robust antiferromagnetism preventing superconductivity in pressurized Ba0.61K0.39Mn2Bi2

Here, we report that K-doped BaMn2Bi2 shows no experimental evidence of superconductivity down to 1.5 K under pressures up to 35.6 GPa, however, a tetragonal to an orthorhombic phase transition is observed at pressure of 20 GPa. Theoretical calculations for the tetragonal and orthorhombic phases, on basis of our high-pressure XRD data, find that the AFM order is robust in both of the phases in pressurized Ba0.61K0.39Mn2Bi2. Our experimental and theoretical results suggest that the K-doped BaMn2Bi2 belongs to a strong Hunds AFM metal with a hybridization of localized spin electrons and itinerant electrons, and that its robust AFM order essentially prevents the emergence of superconductivity.

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arXiv2014

Pressure Induced Superconductivity and Structural Transitions in Ba(Fe0.9Ru0.1)2As2

High pressure electrical resistance and x-ray diffraction measurements have been performed on ruthenium-doped Ba(Fe0.9Ru0.1)2As2, up to pressures of 32 GPa and down to temperatures of 10 K, using designer diamond anvils under quasi-hydrostatic conditions. At 3.9 GPa, there is an evidence of pressure-induced superconductivity with Tc onset of 24 K and zero resistance at Tc zero of ~14.5 K. The superconducting transition temperature reaches maximum at ~5.5 GPa and then decreases gradually with increase in pressure before completely disappearing above 11.5 GPa. Upon increasing pressure at 200 K, an isostructural phase transition from a tetragonal (I4/mmm) phase to a collapsed tetragonal phase is observed at 14 GPa and the collapsed phase persists up to at least 30 GPa. The changes in the unit cell dimensions are highly anisotropic across the phase transition and are qualitatively similar to those observed in undoped BaFe2As2 parent.

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arXiv2014

Complex structures of different CaFe$_{2}$As$_{2}$ samples

The interplay between magnetism and crystal structures in three CaFe$_{2}$As$_{2}$ samples is studied. For the nonmagnetic quenched crystals, different crystalline domains with varying lattice parameters are found, and three phases (orthorhombic, tetragonal, and collapsed tetragonal) coexist between T$_{S}$ = 95 K and 45 K. Annealing of the quenched crystals at 350°C leads to a strain relief through a large (~1.3 %) expansion of the c-parameter and a small (~0.2 %) contraction of the a-parameter, and to local ~0.2 Å displacements at the atomic-level. This annealing procedure results in the most homogeneous crystals for which the antiferromagnetic and orthorhombic phase transitions occur at T$_{N}$/T$_{S}$ = 168(1) K. In the 700°C-annealed crystal, an intermediate strain regime takes place, with tetragonal and orthorhombic structural phases coexisting between 80 to 120 K. The origin of such strong shifts in the transition temperatures are tied to structural parameters. Importantly, with annealing, an increase in the Fe-As length leads to more localized Fe electrons and higher local magnetic moments on Fe ions. Synergistic contribution of other structural parameters, including a decrease in the Fe-Fe distance, and a dramatic increase of the c-parameter, which enhances the Fermi surface nesting in CaFe$_{2}$As$_{2}$, are also discussed.

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arXiv2014

Local inhomogeneity and filamentary superconductivity in Pr-doped CaFe$_{2}$As$_{2}$

We use multi-scale techniques to determine the extent of local inhomogeneity and superconductivity in Ca$_{0.86}$Pr$_{0.14}$Fe$_{2}$As$_{2}$ single crystal. The inhomogeneity is manifested as a spatial variation of praseodymium concentration, local density of states, and superconducting order parameter. We show that the high-$T_{c}$ superconductivity emerges from clover-like defects associated with Pr dopants. The highest $T_{c}$ is observed in both the tetragonal and collapsed tetragonal phases, and its filamentary nature is a consequence of non-uniform Pr distribution that develops localized, isolated superconducting regions within the crystals.

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arXiv2013

High Pressure Effects on the Superconductivity in Rare-Earth Doped CaFe2As2

High-pressure superconductivity in a rare-earth doped Ca0.86Pr0.14Fe2As2 single crystalline sample has been studied up to 12 GPa and temperatures down to 11 K using designer diamond anvil cell under a quasi-hydrostatic pressure medium. The electrical resistance measurements were complemented by high pressure and low temperature x-ray diffraction studies at a synchrotron source. The electrical resistance measurements show an intriguing observation of superconductivity under pressure, with Tc as high as ~51 K at 1.9 GPa, presenting the highest Tc reported in the intermetallic class of 1-2-2 iron-based superconductors. The resistive transition observed suggests a possible existence of two superconducting phases at low pressures of 0.5 GPa: one phase starting at Tc1 ~48 K, and the other starting at Tc2~16 K. The two superconducting transitions show distinct variations with increasing pressure. High pressure low temperature structural studies indicate that the superconducting phase is a collapsed tetragonal ThCr2Si2-type (122) crystal structure. Our high pressure studies indicate that high Tc state attributed to non-bulk superconductivity in rare-earth doped 1-2-2 iron-based superconductors is stable under compression over a broad pressure range.

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arXiv2013

The influence of spin fluctuations on the thermal conductivity in superconducting Ba(Fe_{1-x}Co_x)_2As_2

The thermal conductivity of electron-doped Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$ single crystals is investigated below 200K, with an emphasis on the behavior near the magnetic and superconducting (T_c) transition temperatures. An enhancement of the in-plane thermal conductivity $κ_{ab}$ is observed below T_c for all samples, with the greatest enhancement observed near optimal doping. The observed trends are consistent with the scattering of heat carriers by low-energy magnetic excitations. Upon entering the superconducting state, the formation of a spin-gap leads to reduced scattering and an enhancement in $κ(T)$. Similarly, an enhancement of $κ$ is observed for polycrystalline BaFe2As2 below the magnetic transition, and qualitative differences in $κ(T)$ between single crystalline and polycrystalline BaFe2As2 are utilized to discuss anisotropic scattering. This study highlights how measuring $κ$ near $T_c$ in novel superconductors can be useful as a means to probe the potential role of spin fluctuations.

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arXiv2013

Crystal, magnetic, and electronic structures, and properties of new BaMnPnF (Pn = As, Sb, Bi)

New fluoropnictides BaMnPnF with Pn = As, Sb, Bi, are synthesized by stoichiometric reaction of elements with BaF\_2. The compounds crystallize in the tetragonal P4/nmm (No. 129, Z = 2) space group, with the ZrCuSiAs-type structure, as indicated by single crystal and powder X-ray diffraction results. Electrical resistivity results indicate that Pn = As, Sb, and Bi are semiconductors with band gaps of E\_g = 0.73 eV, E\_g = 0.48 eV and E\_g = 0.003 eV, respectively. Powder neutron diffraction reveals a G-type antiferromagnetic order below T\_N = 338(1) K for Pn = As, and below T\_N = 272(1) K for Pn = Sb. Magnetic susceptibility increases with temperature above 100 K for all the materials. Density functional calculations also find semiconducting antiferromagnetic compounds with strong in-plane and weaker out-of-plane exchange coupling that may result in non-Curie Weiss behavior above T\_N. There is strong covalency between Mn and pnictogen elements. The ordered magnetic moments are 3.65(5) μB/Mn for Pn = As, and 3.66(3) μB/Mn for Pn = Sb at 4 K, as refined from neutron diffraction experiments.

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arXiv2013

Bulk Synthesis of Iron-based Superconductors

Exploratory synthesis efforts for iron-based superconductors (FeSC) have been driven by hopes of improving superconducting critical temperatures (TCs), providing high-quality samples for in-depth studies of intrinsic properties, and exploring potential superconductivity in similar families of materials. This manuscript summarizes the synthesis routes that are used for producing FeSC and their undoped parents, in single crystal and polycrystalline forms. A few of the materials challenges are summarized.

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arXiv2013

Crystals, magnetic and electronic properties of a new ThCr2Si2-type BaMn2Bi2 and K-doped compositions

This is a report on the new 122 ternary transition-metal pnictide of BaMn2Bi2, which is crystallized from bismuth flux. BaMn2Bi2 adopts ThCr2Si2-type structure (I4/mmm) with a = 4.4902(3) Å and c = 14.687(1) Å; it is antiferromagnetic with anisotropic magnetic susceptibility and semiconducting with a band gap of Eg = 6 meV. Heat capacity result confirms the insulating ground state in BaMn2Bi2 with the electronic residual Sommerfeld coefficient of γ ~ 0. The high temperature magnetization results show that magnetic ordering temperature is TN ~ 400 K. Hole-doping in BaMn2Bi2 via potassium in Ba1-xKxMn2Bi2 results in metallic behavior for x = 0.10(1), 0.32(1) and 0.36(1). With K-doping, more magnetically anisotropic behavior is observed. Although there is a downturn in electrical resistivity and low-field magnetization data below 4 K in > 30%-doped crystals, there is no sign of zero resistance or diamagnetism. This manuscript is a report on new materials of BaMn2Bi2 and Ba1-xKxMn2Bi2 (0 < x < 0.4). Results from powder X-ray diffraction, anisotropic temperature- and field-dependent magnetization, temperature-and field-dependent electrical resistivity, and heat capacity are presented.

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arXiv2012

Temperature-composition Phase Diagrams for Ba1-xSrxFe2As2 and Ba0.5Sr0.5(Fe1-yCoy)2As2

Single crystals of mixed alkaline earth metal iron arsenide materials of Ba1-xSrxFe2As2 and Ba0.5Sr0.5(Fe1-yCoy)2As2 are synthesized via the self-flux method. Ba1-xSrxFe2As2 display spin-density wave features (TN) at temperatures intermediate to the parent materials, x = 0 and 1, with TN(x) following an approximately linear trend. Cobalt doping of the 1 to 1 Ba:Sr mixture, Ba0.5Sr0.5(Fe1-yCoy)2As2, results in a superconducting dome with maximum transition temperature of TC = 19 K at y = 0.092, close to the maximum transition temperatures observed in unmixed A(Fe1-yCoy)2As2; however, an annealed crystal with y = 0.141 showed a TC increase from 11 to 16 K with a decrease in Sommerfeld coefficient from 2.58(2) to 0.63(2) mJ/(K2 mol atom). For the underdoped y = 0.053, neutron diffraction results give evidence that TN and structural transition (To) are linked at 78 K, with anomalies observed in magnetization, resistivity and heat capacity data, while a superconducting transition at TC ~ 6 K is seen in resistivity and heat capacity data. Scanning tunneling microscopy measurements for y = 0.073 give Dynes broadening factor of 1.15 and a superconducting gap of 2.37 meV with evidence of surface inhomogeneity.

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arXiv2012

Pressure Induced Superconductivity in Ba0.5Sr0.5Fe2As2

High-pressure electrical resistance measurements have been performed on single crystal Ba0.5Sr0.5Fe2As2 platelets to pressures of 16 GPa and temperatures down to 10 K using designer diamond anvils under quasi-hydrostatic conditions with an insulating steatite pressure medium. The resistance measurements show evidence of pressure-induced superconductivity with an onset transition temperature at ~31 K and zero resistance at ~22 K for a pressure of 3.3 GPa. The transition temperature decreases gradually with increasing in pressure before completely disappearing for pressures above 12 GPa. The present results provide experimental evidence that a solid solution of two 122-type materials, e.g., Ba1-x.SrxFe2As2 (0 < x <1), can also exhibit superconductivity under high pressure

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arXiv2012

Evolution of the nuclear and magnetic structures of TlFe1.6Se2 with temperature

The evolution of the nuclear and magnetic structures of TlFe$_{1.6}$Se$_2$ was determined in the temperature range of 5-450\,K using single crystal neutron diffraction. The Fe layers in these materials develop a corrugation in the magnetically ordered state. A canting away from the block checkerboard magnetic structure is observed in the narrow temperature range between approximately 100 and 150\,K. In this same temperature range, an increase in the corrugation of the Fe layers is observed. At lower temperatures, the block checkerboard magnetic structure is recovered with a suppressed magnetic moment and abrupt changes in the lattice parameters. Microstructure analysis at 300\,K using atomic-resolution Z-contrast scanning transmission electron microscopy reveals regions with ordered and disordered Fe vacancies, and the iron content is found to be uniform across the crystal. These findings highlight the differences between the alkali-metal and thallium materials, and indicate competition between magnetic ground states and a strong coupling of magnetism to the lattice in TlFe$_{1.6}$Se$_2$.

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