The growth by laser ablation and electronic properties of thin cuprate films

In my thesis work I have concentrated on the growth and the in-depth analysis of high temperature superconducting thin films with the central aim to elucidate their electronic properties, predominantly by in-situ angle resolved photoemission spectroscopy (ARPES). I have used two somewhat complementary approaches and two laser ablation set-ups. The first one, developed previously in Wisconsin, was used mainly for studies of strained La2-xSrxCuO4 (LSCO) with a transfer to the Scienta analyzer via an appropriate suitcase. The second one, at the EPFL, where I have built a new pulsed laser deposition (PLD) system, was used to optimize the growth of Bi2Sr2-xLaxCuO4 (Bi-2201) and study in-situ ARPES. In-situ ARPES is the most direct tool to probe the electronic structure. We performed it at the Synchrotron Radiation Center (SRC, University of Wisconsin), where we used the aforementioned experimental set-up consisting in a dedicated PLD system coupled with the SCIENTA beamline. The sample transfer procedure assures that the surface quality is preserved on the way to the SCIENTA analyzer. There we studied in detail the effect of strain in LSCO thin films. In a previous work the in-plane compressive strain was studied and the main result was that the Fermi surface (FS) topology changed from hole-like to electron-like. The tensile strained films showed completely different results. ARPES analysis show evidence for a 3-dimensional (3D) electronic dispersion relation in contrast to the strictly 2-dimensional (2D) dispersion observed in all other studied LSCO films. In this thesis this result has been confirmed mapping the FS at different photon energies. We found that the strain related to the thickness of the films, is playing an important role in inducing a 3D dispersion. Furthermore, the 3D parameters, evolve according to the level of strain. Moreover, we observe a staircase structure for different photon energies, revealing both the 3D nature of the electronic dispersion and the quantization of the electron wave vector along the direction normal to the film surface. Taking advantage of the wavevector quantization we were able to determine directly the band parameters and map the FS without using the nearly-free-electron approximation (NFEA). Moreover, introducing an effective anisotropic photoelectron effective mass, related to the local structure of the excited band, improves the use of the NFEA for single photon energy measurements. In parallel, I have built an improved PLD system at the EPFL which can be connected to the SCIENTA analyzer, and which enables us to perform in-situ ARPES measurements at any time rather than only during allocated beamtimes at the synchrotron. We also produced our own targets for the laser ablation and all the films were fully characterized at the EPFL performing X-ray diffraction (XRD), resistivity and magnetic measurements. I analyzed in detail the growth mechanism of Bi-2201 and I investigated the presence of random intergrowths. We developed a model to explain the presence of these polytypes and studied their presence as a function of the deposition parameters and the annealing treatment. The model predicts a very particular spatial distribution of defects: a Markovian-like sequence of displacements along the grow direction, as well as a two-component in-plane correlation function, characteristic of self-organized intercalates. We varied the growth conditions in order to study the presence of intergrowths and to produce single-phase samples. Subsequently, we performed in-situ photoemission experiments on thin films of Bi-2201 films free from intergrowths and we analyzed their FS. This method is successful and can be extended to other related oxide films.