Fe(Se,Te) Thin Films Deposited through Pulsed Laser Ablation from Spark Plasma Sintered Targets.

Iron-based superconductors are under study for their potential for high-field applications due to their excellent superconducting properties such as low structural anisotropy, large upper critical fields and low field dependence of the critical current density. Between them, Fe(Se,Te) is simple to be synthesized and can be fabricated as a coated conductor through laser ablation on simple metallic templates. In order to make all the steps simple and fast, we have applied the spark plasma sintering technique to synthesize bulk Fe(Se,Te) to obtain quite dense polycrystals in a very short time. The resulting polycrystals are very well connected and show excellent superconducting properties, with a critical temperature onset of about 16 K. In addition, when used as targets for pulsed laser ablation, good thin films are obtained with a critical current density above 105 A cm-2 up to 16 T.

Calorimetric evidence for two phase transitions in Ba1-xKxFe2As2 with fermion pairing and quadrupling states.

Materials that break multiple symmetries allow the formation of four-fermion condensates above the superconducting critical temperature (Tc). Such states can be stabilized by phase fluctuations. Recently, a fermionic quadrupling condensate that breaks the Z2 time-reversal symmetry was reported in Ba1-xKxFe2As2. A phase transition to the new state of matter should be accompanied by a specific heat anomaly at the critical temperature where Z2 time-reversal symmetry is broken ([Formula: see text]). Here, we report on detecting two anomalies in the specific heat of Ba1-xKxFe2As2 at zero magnetic field. The anomaly at the higher temperature is accompanied by the appearance of a spontaneous Nernst effect, indicating the breakdown of Z2 symmetry. The second anomaly at the lower temperature coincides with the transition to a zero-resistance state, indicating the onset of superconductivity. Our data provide the first example of the appearance of a specific heat anomaly above the superconducting phase transition associated with the broken time-reversal symmetry due to the formation of the novel fermion order.

Mechanochemical Synthesis of Sustainable Ternary and Quaternary Nanostructured Cu2SnS3, Cu2ZnSnS4, and Cu2ZnSnSe4 Chalcogenides for Thermoelectric Applications.

Copper-based chalcogenides have emerged as promising thermoelectric materials due to their high thermoelectric performance, tunable transport properties, earth abundance and low toxicity. We have presented an overview of experimental results and first-principal calculations investigating the thermoelectric properties of various polymorphs of Cu2SnS3 (CTS), Cu2ZnSnS4 (CZTS), and Cu2ZnSnSe4 (CZTSe) synthesized by high-energy reactive mechanical alloying (ball milling). Of particular interest are the disordered polymorphs of these materials, which exhibit phonon-glass-electron-crystal behavior-a decoupling of electron and phonon transport properties. The interplay of cationic disorder and nanostructuring leads to ultra-low thermal conductivities while enhancing electronic transport. These beneficial transport properties are the consequence of a plethora of features, including trap states, anharmonicity, rattling, and conductive surface states, both topologically trivial and non-trivial. Based on experimental results and computational methods, this report aims to elucidate the details of the electronic and lattice transport properties, thereby confirming that the higher thermoelectric (TE) performance of disordered polymorphs is essentially due to their complex crystallographic structures. In addition, we have presented synchrotron X-ray diffraction (SR-XRD) measurements and ab initio molecular dynamics (AIMD) simulations of the root-mean-square displacement (RMSD) in these materials, confirming anharmonicity and bond inhomogeneity for disordered polymorphs.

Evidence of the isoelectronic character of F doping in SmFeAsO1-x F x : a first-principles investigation.

We study the electronic structure of the SmFeAsO1-x F x alloy by means of first-principle calculations. We find that, contrary to common believe, F-doping does not change the charge balance between electrons and holes free-carriers in SmFeAsO1-x F x . For energies within a narrow energy range accross [Formula: see text], the effect of F-doping on the band structure dispersion is tiny in both the paramagnetic and stripe antiferromagnetic phase. The charge balance between the conducting FeAs-layer and the SmO1-x F x charge reservoir layer is not influenced by the compositional change. The additional charge carried by fluorine, with respect to the oxygen, is compensated by a change in the oxidation state of the Sm ion from 3+ to 2+. A comparison with the SmFe1-x Co x AsO system shows that such charge compensation by the Sm ion is not shared by donors substituting at the Fe site.

Band filling and disorder effects on the normal state thermoelectric behavior in MgB2.

The goal of this work is providing a comprehensive interpretation framework for the wide and varied experimental phenomenology of the Seebeck effect in MgB2 samples with different levels of doping in either π or σ bands and different levels of disorder, using a combined experimental and theoretical approach. We calculate the temperature dependent diffusive Seebeck coefficient S diff(T) with the Boltzmann equation resolved in relaxation time approximation, taking into account the scattering with phonons and impurities, the effect of renormalization and the effect doping in a rigid band approximation. We show that selective disorder has a sizeable effect on the S diff magnitude, as it tunes the relative contributions of σ and π bands. Disorder also affects the S diff temperature dependences, eventually yielding a linear S diff(T) behavior in the dirty limit. We also show that band filling has opposite effects on S, depending on which band dominates transport. In parallel, we carry out the Seebeck effect measurements on neutron-irradiated Mg11B2, and on two series of doped samples Mg1-x Al x B2 and Mg(B1-x C x )2. From comparison of calculated S diff(T) and experimental S(T) curves, we demonstrate that diffusive and phonon drag terms give comparable contributions in clean samples, but the phonon drag term is progressively suppressed with increasing disorder. In C and Al doped samples we observe very different experimental behaviors in terms of sign, magnitude and temperature dependence. Indeed, notwithstanding the similar electron doping introduced by both substitutions, C or Al doping yields disorder which mainly affects either σ or π bands, respectively. With the help of our theoretical approach, we are able to disentangle the various effects and prove that the Seebeck coefficient is a very sensitive probe of this kind of disorder.

Theoretical and experimental investigation of magnetotransport in iron chalcogenides.

We explore the electronic, transport and thermoelectric properties of Fe1+y Se x Te1-x compounds to clarify the mechanisms of superconductivity in Fe-based compounds. We carry out first-principles density functional theory (DFT) calculations of structural, electronic, magnetic and transport properties and measure resistivity, Hall resistance and Seebeck effect curves. All the transport properties exhibit signatures of the structural/magnetic transitions, such as discontinuities and sign changes of the Seebeck coefficient and of the Hall resistance. These features are reproduced by calculations provided that antiferromagnetic correlations are taken into account and experimental values of lattice constants are considered in DFT calculations. On the other hand, the temperature dependences of the transport properties can not be fully reproduced, and to improve the agreement between experiment and DFT calculations it is necessary to go beyond the constant relaxation time approximation and take into account correlation effects.