Three-dimensional momentum-resolved electronic structure of 1T-TiSe2: A combined soft-x-ray photoemission and density functional theory study

1T-TiSe2 is a quasi-two-dimensional transition metal dichalcogenide, which exhibits a charge density wave transition at a critical temperature of similar to 200 K as well as low-temperature superconductivity induced by pressure or intercalation. The electronic energy dispersion measured by soft x-ray angle-resolved photoemission is not only momentum resolved parallel to the surface but also perpendicular to it. Experiments are compared to density functional theory based band structure calculations using different exchange-correlation functionals. The results reveal the importance of including spin-orbit coupling for a good description of the experimental bands. Compared to calculations within the local density approximation, the use of the modified Becke-Johnson (mBJ) exchange functional leads to a band structure that does not need an artificial downwards shift of the valence band to fit the experiment. The mBJ functional thus clearly appears as the most adapted functional for the theoretical description of the 1T-TiSe2 band structure within the DFT framework.

Spectroscopic Studies on Iron-Chalcogenide Superconductors

Ping-Hui Lin

Superconductivity in F-doped LaFeAsO, Tc= 26 K was first reported by Kamihara et al in 2008. Following that, more iron-based superconductors, e.g., (Ba,K)Fe2As2, LiFeAs, and Fe1+yTe1-xSex were discovered. The new class of high Tc superconductors have attracted a tremendous interest. Iron-chacogenides do not involve arsenic but share several common features with the iron-pnictides. They are characterized by FeCh layers which are isostructural to the FeAs or FeP layers in the iron-pnictides. The electronic structure near the Fermi energy derives from the Fe 3d orbitals. Both families exhibit a spin density wave (SDW) ground state. Se substation for Te in FeTe suppresses the SDW and leads to superconductivity. From a more practical point of view, the iron-chacogenides have a rather simple structure, and they are less toxic and easier to obtain in large single crystals than the arsenide counterparts. For all these properties, the iron-chalcogenides are ideal compounds for angle-resolved photoemission (ARPES) studies. In this thesis, I have investigated by ARPES the normal state electronic structure of Fe1+yTe1-xSex superconductors with various doping level. I have studied the multi-orbital Fermi surface of Fe1+yTe1-xSex, mainly by means of polarized photons from synchrotron radiation sources. Individual bands of different orbital characters could then be distinguished by exploiting ARPES selection rules. I have also investigated the 3D electronic structure of these materials by performing normal emission measurements as a function of the incident photon energy. Namely, by using photon energies as large as 150 eV, I have performed an unusually broad ARPES survey of momentum space. The data reveal two inequivalent Fermi contours at nominally equivalent Gamma points in different Brillouin zones. The observed periodicity corresponds to a unit cell containing only one Fe atom, rather than the standard tetragonal unit cell containing two Fe atoms. I also observe a strong and selective suppression of spectral weight around perpendicular lines at the corner of the Brillouin zone.

EPFL2011

Electrons leave the flatland: out-of-plane charge dynamics in layered materials

Edoardo Martino

The goal of this thesis is to explore the "neglected" third dimension of layered materials, by studying the interlayer charge dynamics through dc conductivity, optical spectroscopy and ab-initio calculations. This project was designed to respond to the growing interest in layered materials and heterostructures. It is today evident that new properties originate by the interaction between neighbouring atomic planes, but the magnitude of the interlayer coupling has so far been poorly investigated. Reliable and reproducible experiments, in particular for dc conductivity, are today made possible thanks to the recent advancements in the field of materials microfabrication through focused ion beam. In the case of this thesis, it enabled me to review long-standing scientific paradigms and verify that previous experimental results differ by more than 2 orders of magnitude from the intrinsic material property. The subjects of study are metallic layered transition metal chalcogenides, as they offer a very flexible playground of crystalline structure and physical properties. The discussion will start in Chapter 3, where we will discuss the case of simple layered metals (2H-NbSe2, 2H-TaS2) or semimetal (ZrTe5), for which the anisotropic transport properties can be accurately predicted by their simple band structure calculation and Fermi surface topology. The anisotropic response will be treated in a more general term by considering the effective number of carriers which contributes to charge transport along a specific direction. The discussion will continue by looking at the peculiar properties of 1T-TaS2, a prominent layered material for the rich set of charge density waves reconstruction, and the presence of a low temperature metal-insulator transition. Recent results from band structure calculations, photoemission spectroscopy and X-ray diffraction, on the contrary, suggests that strong interlayer interactions need to be accounted to justify the observed properties of this material. The experimental results in this thesis provide a clear evidence from transport properties in support of this new interpretation of a layered material where physical properties are strongly dictated by the way different layers interact with each other. This counterintuitive result is regarded as the consequence of the intertwined relation between the charge density wave and the orbital character of the conduction electrons bands, producing a c-axis oriented orbital texture. The weak bond that holds together the crystalline planes in layered materials also creates the perfect condition for intercalation, or the growth of compounds with different crystalline layers stacked together, creating a natural heterostructure. We will explore the new physical properties that emerged in layered transition metal dichalcogenides when different layers are combined together to form a natural heterostructure, or when magnetic ions are intercalated. Surprising results are reported from the studies of interlayer conduction properties. The interaction between the different types of layers in the natural heterostructure of 4Hb-TaS2, influences the charge density wave and superconducting properties. In this situation, the conduction mechanism is highly anisotropic. In Chapter 6 we will see how conduction anisotropy is affected by the specific long-range magnetic order produced by the intercalated atoms.

EPFL2020

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