Static and dynamic spins in superconducting La2-xSrxCuO4: The Riso years

One important area of modern condensed matter research is the investigation of the nature of the superconducting cuprates. Much progress in this field has been obtained with the technique of neutron scattering. We here present a review of neutron scattering studies of the high-temperature superconductor La2-xSrx CuO4, performed at Riso National Laboratory. We review the work on the mapping of the incommensurate spin fluctuations, the investigation of the gap in the fluctuation spectrum, the magnetic properties of the vortices appearing in an applied field, and the quantum critical behaviour of the system. We discuss our findings in the light of results of neutron scattering from other groups, on other cuprate systems, and results from other experimental methods, e.g. NMR, muSR, STM, X-ray diffraction, and ARPES. We end with a discussion on the implications of the experimental results for the progress in the general understanding of high-temperature superconductivity.

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

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

Neutron spectroscopy in the layered quantum magnet SrCu₂(BO₃)₂ and in transition metal phosphorus trisulfides (MPS₃)

Diane Virginie Marie Lançon

Collective magnetic excitations are a fascinating aspect of condensed matter physics, where neutron scattering can provide valuable insight into the magnetic properties of physical realisations of model systems. This thesis focuses on the excitation spectra of layered quantum magnets in the case of the frustrated quantum magnet SrCu

_2

(BO

_3

)

_2

and the family of quasi-2D antiferromagnets MPS

_3

, with M a transition metal. \begin{itemize}[topsep=2pt,itemsep=-0.7ex] \item SrCu

_2

(BO

_3

)

_2

is a physical realisation of the two-dimensional Shastry-Sutherland theoretical model, constructed as orthogonal dimers with the product of singlets on the strong antiferromagnetic

J

bond as an exact ground state. The spin interactions for such a particular geometry induces strong frustration which leads to unconventional magnetism and exotic phases of matter. This work is concerned with a series of aspects of the magnetic excitations in this compound. The excitation spectra as a function of field, temperature and pressure are measured using neutron time-of-flight spectroscopy. The experimental results show that correlations, bound magnons and finite temperature properties are highly unconventional and these results are compared with existing theories on frustrated model systems. In addition, predicted topological properties of SrCu

_2

(BO

_3

)

_2

in an applied field are confirmed experimentally. \item The transition metal phosphorus trisulfides (MPS

_3

) are a family of quasi two-dimensional materials on a honeycomb lattice with weakly bound magnetic planes. This work focuses mainly on the exchange interactions and critical properties of FePS

_3

, which is largely anisotropic with the S=2 Fe

^{2+}

moments pointing normal to the

(a,b)

plane. Inelastic neutron scattering on single crystals is used to measure the spin wave dispersion, providing new insight on the strength of the coupling interactions and anisotropies and showing that FePS

_3

is a good two-dimensional model antiferromagnet. Similar experiments on powdered samples of NiPS

_3

show low-Q dispersive spin waves with a small spin-gap. Critical properties of FePS

_3

close to the Néel temperature are further discussed, as the magnetic nature of the measured quasi-elastic scattering is confirmed. Based on magnetization measurements in high pulsed fields, a possible tricritical point in the 40-50T range is proposed. \end{itemize} The work presented in this thesis has been carried out in a collaboration between the Institut Laue Langevin in Grenoble and the Laboratory for Quantum Magnetism of the EPFL.

EPFL2017