Angle Resolved Photoemission Spectroscopy Studies of the Mott Insulator to Superconductor Evolution in Ca2-xNaxCuO2Cl2

It is widely believed that many of the exotic physical properties of the high-T{sub c} cuprate superconductors arise from the proximity of these materials to the strongly correlated, antiferromagnetic Mott insulating state. Therefore, one of the fundamental questions in the field of high-temperature superconductivity is to understand the insulator-to-superconductor transition and precisely how the electronic structure of Mott insulator evolves as the first holes are doped into the system. This dissertation presents high-resolution, doping dependent angle-resolved photoemission (ARPES) studies of the cuprate superconductor Ca{sub 2-x}Na{sub x}CuO{sub 2}Cl{sub 2}, spanning from the undoped parent Mott insulator to a high-temperature superconductor with a T{sub c} of 22 K. A phenomenological model is proposed to explain how the spectral lineshape, the quasiparticle band dispersion, and the chemical potential all progress with doping in a logical and self-consistent framework. This model is based on Franck-Condon broadening observed in polaronic systems where strong electron-boson interactions cause the quasiparticle residue, Z, to be vanishingly small. Comparisons of the low-lying states to different electronic states in the valence band strongly suggest that the coupling of the photohole to the lattice (i.e. lattice polaron formation) is the dominant broadening mechanism for the lower Hubbard band states. Combining this polaronic framework with high-resolution ARPES measurements finally provides a resolution to the long-standing controversy over the behavior of the chemical potential in the high-T{sub c} cuprates. This scenario arises from replacing the conventional Fermi liquid quasiparticle interpretation of the features in the Mott insulator by a Franck-Condon model, allowing the reassignment of the position of the quasiparticle pole. As a function of hole doping, the chemical potential shifts smoothly into the valence band while spectral weight is transferred from incoherent weight at high energies to a coherent quasiparticle peak near E{sub F}. The combined shift in the chemical potential and Fermi wavevector, k{sub F}, closely corresponds to a rigid band shift into the faint excitation branch defined by the low-energy quasiparticles. In addition, the detailed doping evolution of the low-energy excitations has been studied throughout k-space. A large, hole-like contour emerges with doping, although well-defined quasiparticle peaks are only observed along a small arc around the (0, 0)-({pi},{pi}) nodal line. Near the ({pi}, 0) antinodes, faint parallel segments are found with a nesting wavevector and energy dependence very similar to the 4a{sub 0} x 4a{sub 0} checkerboard pattern observed by scanning tunneling microscopy. However, these measurements reveal a striking dichotomy between the real and momentum-space probes, where antinodal charge ordering is emphasized in the tunnelling measurements, while ARPES is most sensitive to excitations near the d-wave nodal line. These results emphasize the importance of momentum anisotropy in determining the complex electronic properties of the cuprates and places strong constraints on theoretical models of the charge ordered state