Adatoms, Quasiparticles & Photons The Multifaceted World of Photoelectron Spectroscopy

University dissertation from Stockholm : KTH

Abstract: The experimental work presented in this thesis is based on a wide assortment of very advanced and highly sophisticated photoelectron spectroscopy (PES) techniques. The objective of the present study has been to reveal and understand the electronic structure and electron dynamics in a broad spectrum of materials, ranging from wide band gap oxides, via semiconductors along with metals, and finally high-temperature superconductors.The first part of the thesis concerns laser-based pump-and-probe PES. This unique experimental technique has permitted a study of the excited electronic structure and the electron dynamics of several semiconductor surfaces. An insight into details of the adatom to restatom charge-transfer of the Ge(111)c(2x8) surface is presented, as well as an estimate for the timescale in which the dynamic adatoms of the Ge(111):Sn(sqrt3xsqrt3)R30deg surface operate. Further results comprise a novel unoccupied surface state at the GaSb(001) surface as well as a time-resolved study of the charge accumulation layer at the InAs(111)A/B surfaces.In the second part, high-resolution synchrotron based angle-resolved PES (ARPES) data from the cuprate high-temperature superconductor La(2-x)Sr(x)CuO(4) (LSCO) is presented. This extensive study, reveals detailed information about how the Fermi surface and electronic excitations evolve with doping in the superconducting state. The results comprise support for a connection between high- and low-energy electronic responses, the characteristics of the superconducting gap, and indication of a quantum phase transition between two different superconducting phases.In the third group of experiments we move away from the two-dimensional systems and concentrate on fully three-dimensional compounds. By the use of soft x-ray ARPES it is possible to extract the three-dimensional electronic structure in a straightforward manner with increased k(perpendicular)-resolution. As a result the first high-quality ARPES data from Cu2O is presented, as well as a novel method for extracting the (real space) electron density by ARPES. These experiments clearly display the advantages of using soft x-ray ARPES. If the material and type of experiment is chosen wisely, the benefit of the increased k||-window and the free electron final state, surpass the drawbacks of decreased count-rate and inferior energy resolution. Finally we return to the high-temperature superconductors (NCCO & Nd-LSCO) and make use of the increased bulk-sensitivity. From an evident change in the shape of the Fermi surface when moving from low to high photon energies, the durface to bulk difference in electronic structure is highlighted.

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