Single-particle spectroscopic probes, such as scanning tunneling and angle-resolved photoemission spectroscopy (ARPES), have provided us with crucial insights into the complex electronic structure of the high-Tc cuprates, in particular for the under and optimally doped regimes where high-quality crystals suitable for surface-sensitive experiments are available. Conversely, the elementary excitations on the heavily overdoped side of the phase diagram remain largely unexplored. Important breakthroughs could come from the study of Tl2Ba2CuO6+d (Tl2201), a structurally simple system whose doping level can be tuned from optimal to extreme overdoping by varying the oxygen content. We have grown single crystals of Tl2201, which were then carefully annealed under controlled oxygen partial pressures. Their high quality and homogeneity are demonstrated by narrow rocking curves and superconducting transition widths. These crystals have enabled the first successful ARPES study of both normal and superconducting-state electronic structure in Tl2201, allowing a direct comparison with the Fermi surface from magnetoresistance and the gap from thermal conductivity experiments. This establishes Tl2201 as the first high-Tc cuprate for which a surface-sensitive single-particle spectroscopy and a comparable bulk transport technique have arrived at quantitative agreement on a major feature such as the normal state Fermi surface. The surprising momentum dependence of the ARPES lineshape is also discussed.
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