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Register a new userStructural anomaly in superconductivity of CaFe2As2 class of materials
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Added by
Prof. Kalobaran Maiti
Publication date
2020
fields
Physics
and research's language is
English
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Quantum transitions in Fe-based systems are believed to involve spin, charge and nematic fluctuations. Complex structural phase diagram in these materials often emphasizes importance of covalency in their exotic properties, which is directly linked to the local structural network and barely understood. In order to address this outstanding issue, we investigate the evolution of structural parameters and their implication in unconventional superconductivity of 122 class of materials employing extended x-ray absorption fine structure studies. The spectral functions near the Fe K- and As K-absorption edge of CaFe2As2 and its superconducting composition, CaFe1.9Co0.1As2 (Tc = 12 K) exhibit evidence of enhancement of Fe contribution with Co-substitution near the Fermi level. As-Fe and Fe-Fe bondlengths derived from the experimental data exhibit interesting changes with temperature across the magneto-structural transition. Curiously, the evolution in Co-doped composition is similar to its parent compound despite absence of magneto-structural transition. In addition, we discover anomalous change of Ca-X (X = Fe, As) bondlengths with temperature in the vicinity of magneto-structural transition and disorder appears to be less important presumably due to screening by the charge reservoir layer. These results reveal evidence of doping induced evolution to the proximity to critical behavior presumably leading to superconductivity in the system.
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Aliovalent rare earth substitution into the alkaline earth site of CaFe2As2 single-crystals is used to fine-tune structural, magnetic and electronic properties of this iron-based superconducting system. Neutron and single crystal x-ray scattering experiments indicate that an isostructural collapse of the tetragonal unit cell can be controllably induced at ambient pressures by choice of substituent ion size. This instability is driven by the interlayer As-As anion separation, resulting in an unprecedented thermal expansion coefficient of $180times 10^{-6}$ K$^{-1}$. Electrical transport and magnetic susceptibility measurements reveal abrupt changes in the physical properties through the collapse as a function of temperature, including a reconstruction of the electronic structure. Superconductivity with onset transition temperatures as high as 47 K is stabilized by the suppression of antiferromagnetic order via chemical pressure, electron doping or a combination of both. Extensive investigations are performed to understand the observations of partial volume-fraction diamagnetic screening, ruling out extrinsic sources such as strain mechanisms, surface states or foreign phases as the cause of this superconducting phase that appears to be stable in both collapsed and uncollapsed structures.
The structural properties of the CaFe2As2 have been investigated by x-ray and neutron powder diffraction techniques as a function of temperature. Unambiguous experimental evidence is shown for coexistence of tetragonal and orthorhombic phases below 170 K in contrast to existing literature. Detailed Rietveld analyses of thermo-diffractograms show that the sample does not transform completely in to the orthorhombic phase at the lowest temperature even though it is the majority phase. We have found that the unit cell volume of the orthorhombic phase is higher compared to that of the tetragonal phase for all the temperatures. X-ray data on CaFe2As2 shows anomalous (at) lattice parameter contraction with increasing temperature and phase co-existence behavior below 170 K unlike other members of the 122 family of compounds like SrFe2As2 and EuFe2As2. Temperature dependent magnetization of polycrystalline CaFe2As2 sample show weak anomalies below 170 K. This behavior of the polycrystalline sample is in contrast to that of a single crystal reported earlier.
We studied the effect of hydrostatic pressure (P) on the structural phase transitions and superconductivity in the ternary and pseudo-ternary iron arsenides CaFe2As2, BaFe2As2, and (Ba0.55K0.45)Fe2As2, by means of measurements of electrical resistivity (rho) in the 1.8 - 300 K temperature (T) range, pressures up to 20 kbar, and magnetic fields up to 9 T. CaFe2As2 and BaFe2As2 (lightly doped with Sn) display structural phase transitions near 170 K and 85 K, respectively, and do not exhibit superconductivity in ambient pressure, while K-doped (Ba0.55K0.45)Fe2As2 is superconducting for T < 30 K. The effect of pressure on BaFe2As2 is to shift the onset of the crystallographic transformation down in temperature at the rate of about -1.04 K/kbar, while shifting the whole rho(T) curves downward, whereas its effect on superconducting (Ba0.55K0.45)Fe2As2 is to shift the onset of superconductivity to lower temperatures at the rate of about -0.21 K/kbar. The effect of pressure on CaFe2As2 is first to suppress the crystallographic transformation and induce superconductivity with onset near 12 K very rapidly, i.e., for P < 5 kbar. However, higher pressures bring about another phase transformation characterized by reduced resistivity, and the suppression of superconductivity, confining superconductivity to a narrow pressure dome centered near 5 kbar. Upper critical field (Hc2) data in (Ba0.55K0.45)Fe2As2 and CaFe2As2 are discussed.
The structural properties of the SrFe2As2 and CaFe2As2 compounds have been extensively analyzed by transmission electron microscopy (TEM) from room temperature down to 20K. The experimental results demonstrate that the SrFe2As2 crystal, in consistence with previous x-ray data, has a tetragonal structure at room temperature and undergoes a tetragonal (T)-orthorhombic (O) phase transition at about 210K. Moreover, twinning lamella arising from T-O transition evidently appears in the orthorhombic phase. On the other hand, TEM observations of CaFe2As2 reveal the presence of a pseudo-periodic structural modulation with the periodicity of around 40nm at room temperature. This modulation is likely in connection with the local structural distortions within the Ca layer. In-situ cooling TEM observations of CaFe2As2 reveal the presence of complex domain structures in the low-temperature orthorhombic phase.
75As-zero-field nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements are performed on CaFe2As2 under pressure. At P = 4.7 and 10.8 kbar, the temperature dependences of nuclear-spin-lattice relaxation rate (1/T1) measured in the tetragonal phase show no coherence peak just below Tc(P) and decrease with decreasing temperature. The superconductivity is gapless at P = 4.7 kbar but evolves to that with multiple gaps at P = 10.8 kbar. We find that the superconductivity appears near a quantum critical point under pressures in the range 4.7 kbar < P < 10.8 kbar. Both electron correlation and superconductivity disappear in the collapsed tetragonal phase. A systematic study under pressure indicates that electron correlations play a vital role in forming Cooper pairs in this compound.
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