Pressure induced evolution of superconductivity and magnetic hourglass dispersion in Fe1.02Te0.7Se0.3

Iron based high temperature superconductors have several common features with superconducting cuprates, including the square lattice and the proximity to an antiferromagnetic phase. The magnetic excitation spectrum below T-c of Fe1.02Te0.7Se0.3 shows an hourglass-shaped dispersion with a resonance around the commensurate point. In a previous inelastic neutron scattering study, we showed that the hourglass-shaped dispersion is most likely a prerequisite for superconductivity, while the consequences are the opening of a gap and a shift of spectral weight. In this paper we follow the evolution of the hourglass shaped dispersion under applied pressure up to 12 kbar. Our results show that that the pressure-induced 37% increase of T-c is concomitant with a change in the magnetic excitation spectrum, with an increase of the hourglass energy by 38%.

Normal state transport properties of novel superconductors

Balazs Sipos

The discovery of high temperature superconductivity in the cuprates in 1986 has boosted the research in strongly correlated materials. One strong motivation was and stays the understanding the high-Tc phenomenon with the hope that one can ultimately engineer new materials with even higher Tc. Besides the in-depth investigation of cuprates, there is a strong tendency in the solid state community to find new superconductors, which by themselves are interesting for applications, or by their properties they can contribute to the understanding of the high-Tc phenomenon. The program of my doctoral thesis was three-fold: i) to address one important issue in the cuprate superconductors, that of the role of homogeneity in the underdoped part of the phase diagram; ii) what is the effect of disorder in MgB2 superconductor, which has high potentials for applications; iii) to discover new superconductors in the family of transition metal dichalcogenides. All these materials are in some sense unconventional superconductors. The cuprates by their high Tc and the symmetry of the order parameter, MgB2 by its two-band superconductivity and Tc of 39 K, and the dichalcogenides by the appearance of superconductivity on the background of competing interactions. Measurements of transport properties, such as resistivity and thermoelectric power, were used to get insight in the behavior of these materials. Besides temperature as variable, I applied high pressure, extreme magnetic fields and controlled disorder introduced by fast electron irradiation. In the first part I present the pressure dependent study of two members of the transition metal dichalcogenides having 1T structure, 1T-TiSe2 and 1T-TaS2, where superconductivity was never observed in a pristine sample. 1T-TiSe2 has a CDW phase below 220 K which origin, weather it is driven by an excitonic mechanism or by a Jahn-Teller distortion, is an ongoing question. By applying pressure I showed that the pristine sample is superconducting in the pressure range of 2.0–4.0 GPa. This range remarkably coincides with the short range fluctuating CDW before its disappearance at the upper pressure value. If CDW is due to excitonic interactions than our observations suggest that it can be at the origin of superconductivity, as well. The second dichalcogenide is the 1T-TaS2, where a Mott-insulator phase appears on the top of a commensurate CDW. By applying pressure I was able to melt that Mott-phase, and reveal that the material is superconducting above 2.5 GPa with Tc of 5.9 K. Unexpectedly, superconductivity is born from a nonmetallic phase, and stays remarkably stable up to the highest applied pressure of 24 GPa. In the second part I tried to give my contribution to the field of high-Tc superconductors. I carefully selected few high quality underdoped Bi2Sr2PrxCa1-xCu2O8-δ sample, to address the nature of the low temperature ground state by applying high magnetic field. Although former measurements by other groups showed that at high underdoping, the ground state is an insulator, I found that a sample with as low Tc as 15 K exhibits metallic behavior up to 60 T. Furthermore, I showed that a inhomogeneous distribution of the doping atoms can completely mask the intrinsic normal state of a high-Tc superconductor. In the last part of my thesis I focused on the two-band superconductor MgB2 by studying the scattering between the bands by the means of the Matthiessen's rule. I made a systematic study of the influence of defects created by fast electron irradiation, and found that the the Matthiessen's rule is satisfied for the defect concentration range I induced. I further compare the influence of defects on the critical temperature and the residual resistivity in MgB2 with superconductors with various order parameters, and found that the decrease-rate of Tc in our system is within the range of a response of a superconductor with an s-wave order parameter.

EPFL2008

Thermopower as a Unique Tool to Probe Quantum Phase Transitions

Stevan Arsenijevic

In my thesis, transport measurements such as resistivity and, more importantly, thermopower S, were used to explore the phase diagram of bad metals. Bad metals are electronically correlated systems whose ground state lies close to a quantum phase transition. By tuning the control parameters, such as temperature (T ), magnetic field (B), hydrostatic pressure (p) or chemical substitution (x), we can induce phase transitions between the various electronic, magnetic and structural phases. Here, the thermopower is presented as a unique tool for probing quantum phase transition because it is a measure of the entropy of conducting electrons. The main part of the thesis is dedicated to the study of Fe-based superconductors (FeSC) discovered in 2008. Their parent compound has an antiferromagnetic (AF) ground state, where the itinerant electrons form a spin-density wave (SDW), a periodic modulation of spin density. This coincides or is preceded by a structural, tetragonal-to-orthorhombic transition. The nesting between the electron and hole Fermi surface is believed to be the driving mechanism for the SDW state. By changing the structural or chemical properties the AF ground state of FeSC is suppressed, giving way to superconductivity (SC). The remaining antiferromagnetic fluctuations above the transition can provide a glue for SC pairing. Here, the analysis of the thermopower S/T of BaFe1−xCoxAs2 (BFCA) in the x-T phase diagram shows the signatures of the spin fluctuation which have a dome-like dependence and follow the trend of superconducting Tc . The logarithmic increase of S/T upon decreasing T is ascribed to the proximity of the spin-density-wave quantum critical point. It can be understood as an increase of entropy due to the incommensurate AF spin fluctuations. We can ascribe the high values of thermopower in BFCA at intermediate- and room-temperatures to the influence of low-T quantum criticality. To probe the response of the electronic system in FeSC to structural changes, we performed measurements under pressure of the parent compound BaFe2As2 (BFA), the SC electron-doped BFCA, and hole-doped Ba1−xKxFe2As2 (BKFA). In the parent compound pressure suppresses the structural/SDW transition, similar to the effect of doping. For doped systems, in order to describe the behavior of thermopower in the high-T range (above 100K) we used a semi-metallic two-band model which was fitted to the data in order to extract the pressure dependence of the band parameters. In both doping cases the effect of pressure was similar, an increase of the band overlap and of the effective number of charge carriers. With this model we can explain the high-T , x and p dependence of thermopower in both electron- and hole-doped BFA. In a structurally simpler Fe-chalcogenide Fe1+yTe1−xSex compound, the excess of Fe has a Kondo-like influence on the charge carriers which dramatically changes the physics of the normal state. To probe the normal state, pressure, doping, magnetic Fe-excess concentration (y) and temperature were used as control parameters. At low-T a characteristic upturn of resistivity (ρmag ) is observed, followed by an increase of thermopower (Smag ), which we identify as the magnetic contribution caused by the spin-flip scattering events. Increasing the y resulted in an increase of ρmag , and a decrease of Smag , which is in agreement with the behavior of canonical Kondo-systems. Pressure suppresses the magnetic contribution to transport, thus increasing the itinerancy of the system. MnSi is another system in which the sensitivity of thermopower to entropy brings new information related to the complex magnetic structure. Pressure was used to drive the system from a helically ordered, canonical Fermi-liquid (FL) phase with T 2-resistivity to the intrinsically disordered, non-Fermi-liquid (NFL) phase above pc with T3/2-dependence. Our contour plot of S/T demonstrated how powerful the thermopower technique is, by reproducing the whole previously established T -p phase diagram. At the phase transition from the magnetically-ordered FL phase to the disordered NFL, the thermopower is dramatically enhanced. We bring useful information about the mysterious partial order (PO) phase inside the NFL phase, previously detected only by neutron scattering. The fluctuating helices scenario can describe the observed increase of entropy/thermopower in the PO phase. At ambient pressure, close to the helical transition of MnSi, a moderate magnetic field can stabilize the skyrmion lattice - the lattice of topological magnetic whirls, vortices. We observe a signature of the skyrmion lattice as a minute drop in thermopower. It is located exactly in the same region of the T − B phase diagram where an increase in magnetoresistance and Hall effect was reported previously. This feature originates from the additional scattering of conducting electrons on magnetic vortices, while the change in S is dominated by the decrease of entropy as the stable skyrmion lattice is formed. Overall, resistivity was used to confirm the established phase diagram, while thermopower, as an interesting and not sufficiently understood technique, was used to probe the sensitive changes of the charge carriers at the Fermi surface. We explored various phases showing how useful thermopower is to probe the entropy of electronic system on the verge of quantum phase transition.

EPFL2012

The Interplay Between Structural and Electronic Degrees of Freedom in Superconductors

Mathieu Julien Gino Cottet

More than one hundred years after the discovery of superconductivity in Leiden, the intriguing physics of several unconventional classes of superconductors continue to fascinate and challenge scientists from all over the world. The majority of these compounds belongs to a major class of materials known as strongly correlated systems that exhibit interesting and diverse physical properties, like the high-temperature superconductivity, the Mott-insulator transition, the colossal magnetoresistance or the structurally-driven electronic phase transitions. Rigorous and deep investigations of the electronic properties, as well as their tunability, should lead to new attractive commercial applications. With the use of time-resolved experiments or bulk sensitive techniques, which represent the main subject of this thesis, the electronic and magnetic properties of strongly correlated type-II superconductors and high-temperature copper-oxide superconductors are accessible. These techniques take advantages of the photon tunability in the case of optical pump-probe by allowing one to record the transient response of the material over the whole visible spectrum, or in the case of X-ray diffraction, the tunability of the synchrotron radiation thanks to the slicing operating at the SLS (Swiss Light Source) in Villigen, Switzerland. Cryo-LTEM allows one to work across the (H ,T ) phase diagram of type-II superconductors, thus enabling the study of the coexistence between normal and superconducting state by careful regulation of the applied magnetic field near the specimen. The Chapter 1 (1) is a general introduction dedicated to the historical evolution of our understanding of superconductivity, according to the theories and general concepts used and developed is this thesis. Chapter 2 (3) is dedicated to the experimental techniques. A careful description of the different setups, as well as a theoretical development needed for the calculations is presented. In Chapter 3 (4), the investigation of magnesium diboride superconductor by means of cryo-LTEM is presented. By observing the field-dependent vortex lattices in this system and performing calculations using the theoretical frameworks developed by Ginzburg-Landau and Abrikosov, I found that this compound belongs to the type-II family [1], and not to the novel type 1.5 class of superconductor. In Chapter 4 (5), I present the investigation related the charge density waves compound Lu5Ir4Si10. The use of ultrafast time-resolved optical pump-probe experiments, coupled with ab-anitio theoretical calculations of the electron-phonon coupling and the electronic structure, permits to shine new light on the nature of this transition which we identified as a structurally-driven Peierls transition [2]. The Chapter 5 (6) is dedicated to the investigation of the high-temperature copper-oxide superconductor, La2−x Srx CuO4, for different doping levels; the experiment was carrying out at the SLS on the Micro-XAS beamline, By using a transient temperature model and comparing our experimental results with temperature-dependent density of states calculations, we report on the electronic temperature dependence of the electron-phonon coupling constant (submitted to Phys. Rev. B).

EPFL2013