Resonant Inelastic X-Ray Scattering Study of Electron-Exciton Coupling in High-T-c Cuprates

Explaining the mechanism of superconductivity in the high-T-c cuprates requires an understanding of what causes electrons to form Cooper pairs. Pairing can be mediated by phonons, the screened Coulomb force, spin or charge fluctuations, excitons, or by a combination of these. An excitonic pairing mechanism has been postulated, but experimental evidence for coupling between conduction electrons and excitons in the cuprates is sporadic. Here we use resonant inelastic x-ray scattering to monitor the temperature dependence of the dd exciton spectrum of Bi2Sr2CaCu2O8-x crystals with different charge carrier concentrations. We observe a significant change of the dd exciton spectra when the materials pass from the normal state into the superconductor state. Our observations show that the dd excitons start to shift up (down) in the overdoped (underdoped) sample when the material enters the superconducting phase. We attribute the superconductivity-induced effect and its sign reversal from underdoped to overdoped to the exchange coupling of the site of the dd exciton to the surrounding copper spins.

Dynamics and coherent effects on high density plasmas in semiconductor nanostructures

Lars Kappei

This thesis work contains an experimental study of many-body and cooperative effects in quantum wells. Many-body effects prove important for an understanding of the physical and specifically optical properties of semiconductors. The Coulomb interaction between electrons profoundly modifies the electronic states and the light-matter interaction, leading to a number of density-dependent effects that can not be accounted for in the one-electron picture which is the starting point of most textbooks on the subject. The simplest of these modifications is the exciton, the bound state of one electron and one hole which leads to the emergence of two-particle states energetically below the continuous band electron-hole states. Optical excitation in the band continuum is possibly followed by the formation of excitons upon release of the excess energy to the lattice vibrations. Chapter 5 contains an experimental analysis of the dynamics of this process. A high quality single In0.05Ga0.95As/GaAs quantum well sample allows us to separately study the temporal evolution of the continuum photoluminescence on the one hand and the excitonic photoluminescence on the other. The results indicate a rather fast formation process, leading to the establishment of a species interconversion equilibrium between free pairs and bound pairs at higher density. However, at the lowest excitation density, we found evidence for a non-equilibrium species repartition. At high electron-hole pair density, the two-particle bound exciton state disappears due to the screening of the Coulomb interaction by the surrounding carriers as well as the blocking of the constituting states according to the Pauli exclusion principle. The transition from an excitonic population to a free carrier plasma is referred to as excitonic Mott transition. Chapter 6 reports an experimental investigation of the repercussions of this transition on the optical spectra, performed on the In0.05Ga0.95As/GaAs quantum well of chapter 5. The time-resolved spectra do not show an abrupt change of photoluminescence intensity or spectral form when transforming gradually from an exciton dominated spectrum to free plasma photoluminescence, indicating a rather gradual transition. The separate visibility of continuum and excitonic PL contributions below the transition density reveals the total absence of exciton binding energy variations, indicating a very low exciton ionization degree in contrast to theoretical work on the subject. Another high-density effect arising from the particle interactions is the energetic lowering of the electronic states due to screening and correlation, denoted as band gap renormalization (BGR). Chapter 7 presents measurements of BGR using a single GaAs/Al0.25Ga0.75As quantum well of 60 Å width. We obtain good agreement with calculations of the carrier self energy within the framework of the random phase approximation. The last part of this thesis (chapter 8) reports an experimental test of the possibility of cooperative spontaneous emission, often denoted as superradiance, from a high-density electron-hole plasma. This effect has been extensively studied in optically excited atomic gases, where it leads under certain conditions to the reemission of the stored energy in a single coherent radiation burst instead of the slow exponential decay according to the spontaneous radiation of a single atom. We find no evidence for the occurrence of this effect in our samples, probably due to the fast incoherent polarization decay in the carrier plasma.

EPFL2005

Pressure-tuned Transport Properties of Novel Iron-based Superconductors and Topological Insulators

Andrea Pisoni

The majority of interactions in solids strongly depend on the interatomic distances. The application of pressure changes the lattice parameters and modifies the electronic and the phononic energy spectra of a material avoiding some of the undesirable effects induced by chemical doping, like lattice disorder, impurity phases and phase separations. Layered materials are particularly affected by the application of pressure because their anisotropic structure eases the contraction of the lattice along specific crystallographic directions. In this thesis I study the effect of pressure on the transport properties of two new layered materials: L4Fe2As2Te(1-x)O4 (L = Pr, Sm, Gd) superconductors and beta-Bi4I4 topological insulator. The discovery of Fe-based superconductors (Fe-SCs) provided a new material base for studying the mechanism of high temperature superconductivity. These materials present unexpectedly high critical temperatures (Tc ) despite the presence of magnetic atoms. The parent compounds of Fe-SCs are semimetals with an antiferromagnetic ground state in which the itinerant electrons form a periodic modulation of spin density called spin density wave (SDW). By changing the structural properties or by adding/removing carriers the SDW order can be suppressed and superconductivity emerges. Our group recently succeeded in synthesizing a new family of Fe-SCs that presents Tc up to 45 K upon optimum chemical doping and substitution. I performed a systematic study of the upper critical field and the pressure-dependent electrical resistivity of single crystals of Pr4Fe2As2Te(1-x)O4 and Sm4Fe2As2Te(1-x)O(4-y)Fy . Hall coefficient and magnetoresistance of Pr4Fe2As2Te(1-x)O4 revealed electrons as the dominant type of charge carriers. The results can be successfully fitted by a two-band model that allows the estimation of the temperature dependent electron and hole densities and mobilities. In view of the exceptionally high structural anisotropy of this new class of Fe-SCs I investigated the electronic anisotropy of Sm4Fe2As2Te(1-x)O(4-y)Fy by means of microfabrication techniques. The results show a ratio between the out-of-plane and in-plane electrical resistivities that is the highest reported so far in Fe-SCs. Topological insulators (TIs) form another class of materials that is currently attracting a lot of attention both for fundamental physics and potential applications. In TIs metallic surface states coexist with an insulating bulk. Most of the TIs known so far are either three-dimensional strongly bonded bulk materials or layered van der Waals crystals. Beta-Bi4I4 is a material composed of quasi-one-dimensional molecular chains that was theoretically predicted, and only recently experimentally verified, to be a novel strong topological insulator. Due to its particular structure, beta-Bi4I4 offers the possibility to study the interplay between different ground states like topological insulating phase, charge-density-wave and superconductivity. Here I present, for the first time, a study of the thermoelectric properties of beta-Bi4I4 single crystals. Electrical resistivity, Seebeck coefficient, thermal conductivity and Hall coefficient measurements reveal a possible charge density-wave-order (CDW) at low temperature. According to resistivity and thermoelectric power measurements, pressure suppresses the CDW order. Resistivity measurements performed in a diamond anvil cell up to 20 GPa demonstrate that superconductivity is induced in beta-Bi4I4 for pressure above 10 GPa. Preliminary X-ray diffraction measurements by synchrotron radiation, performed on the sample recovered at ambient pressure after the experiment, reveal that a new Bi-I phase is formed at high pressure. The possibility that the topological insulator state could coexist with superconductivity in beta-Bi4I4 is certainly a fascinating option but it remains for now an open question.

EPFL2016

Kinks in the angle resolved photoemission and inelastic x-ray spectra of high temperature superconductors

Jeff Graf

Though the high superconducting transition temperature (Tc) is the most interesting technological aspect of high temperature superconductors, the complex way in which the spin, lattice and electronic degrees of freedom interplay, makes them of the highest scientific interest. This is illustrated by their rich phase diagram characterized by a variety of exotic groundstate including; Mott insulating, pseudogap and high temperature superconductivity. One of the most serious barriers that has prevented our understanding of the mechanism of high temperature superconductors thus far is the lack of information on how low energy Landau quasiparticles result from an organization of real particles. This organization, often colloquially referred to as "dressing", is a fundamental general concept in physics that explains a variety of physical phenomena, such as exotic particle formations and phase transitions. The role of the lattice in this dressing is particularly controversial. Phonons are quanta of lattice vibration energy, and play a crucial role in conventional superconductivity. They provide an attractive interaction allowing the electrons to condensate in superconducting Cooper pairs. However, high temperature superconductivity in the cuprates in achieved through hole doping in an antiferromagnetic Mott insulator. In this case, the antiferromagnetic background, the strong coulomb repulsion and the anisotropic superconducting gap all suggest a marginal role of the phonons. In order to assess experimentally the exact role of the phonon, angle resolved photoemission spectroscopy (ARPES) is the weapon of choice given its unique ability to probe the electronic structure of solids in an energy- and momentum-resolved manner. In this thesis, I will use ARPES to characterize the various form of dressing of the quasiparticles in the high temperature superconductor from the Fermi level all the way to the valence band complex. I'll show that when combined with isotope substitution and inelastic x-rays scattering, the strong electron-phonon interaction can be probed in vivid details. This thesis presents three fundamental results. 1) Using the isotope effect, the important and unusual role of the phonon is demonstrated, as well as the strong interplay between the magnetic and phonic degrees of freedom. 2) Using inelastic scattering, the intriguing interplay between the Fermi surface and the bond stretching phonon is exposed. And 3) By exploring the ARPES data up to high energy, two new energy scales at high binding energy as well as the spectral waterfalls phenomenon are revealed. When all these new elements are considered together, they clearly show the need to consider simultaneously the spin, lattice, Fermi surface topology and electronic degrees of freedom. The spectacular progress in ARPES techniques over the past two decades was critical for these results, and I will present in this thesis our current effort in pushing the techniques even further. In particular I'll present my efforts in building a laser based ARPES setup with a hemispherical analyzer and a spin resolved time of flight analyzer.

EPFL2008