Visualizing the Interplay of Structural and Electronic Disorders in High-Temperature Superconductors Using Scanning Tunneling Microscopy

The discovery of high-$T_c$ superconductivity in 1986 generated tremendous excitement. However, despite over 25 years of intense research efforts, many properties of these complex materials are still poorly understood. For example, the cuprate phase diagram is dominated by a mysterious "pseudogap" state, a depletion in the Fermi level density of states which persists above the superconducting critical temperature $T_c$. Furthermore, these materials are typically electronically inhomogeneous at the atomic scale, but to what extent the intrinsic chemical or structural disorder is responsible for electronic inhomogeneity, and whether the inhomogeneity is relevant to pseudogap or superconductivity, are unresolved questions. In this thesis, I will describe scanning tunneling microscopy experiments which probe the interplay of structural, chemical and electronic disorder in high-$T_c$ superconductors. First, I will present the imaging of a picoscale orthorhombic structural distortion in Bi-based cuprates. Based on insensitivity of this structural distortion to temperature, magnetic field, and doping level we conclude that it is an omnipresent background not related to the pseudogap state. I will also present the discovery of three types of oxygen disorder in the high-$T_c$ superconductor $Bi_2Sr_2CaCu_2O_{8+x}$ two different interstitials as well as vacancies at the apical oxygen site. We find a strong correlation between the positions of these defects and the nanoscale inhomogeneity in the pseudogap phase, which highlights the importance of chemical disorder in these compounds. Furthermore, I will show the determination of the exact intra-unit-cell positions of these dopants and the effect of different types of intrinsic strain on their placement. I will also describe the identification of chemical disorder in another cuprate $Y_{1−x}Ca_xBa_2Cu_3O_{7−x}$, and the first observation of electronic inhomogeneity of the spectral gap in this material. Finally, I will present definitive identification of the cleavage surfaces in $Pr_xCa_{1−x}Fe_2As_2$, and imaging of Pr dopants which exhibit lack of clustering, thus ruling out Pr inhomogeneity as the likely source of the high-$T_c$ volume fraction. To achieve the aforementioned results, we employ novel analytical and experimental tools such as an average supercell algorithm, high-bias dI/dV dopant mapping, and local barrier height mapping.Physic

Interplay of chemical disorder and electronic inhomogeneity in unconventional superconductors

Many of today's forefront materials, such as high-Tc superconductors, doped semiconductors, and colossal magnetoresistance materials, are structurally, chemically and/or electronically inhomogeneous at the nanoscale. Although inhomogeneity can degrade the utility of some materials, defects can also be advantageous. Quite generally, defects can serve as nanoscale probes and facilitate quasiparticle scattering used to extract otherwise inaccessible electronic properties. In superconductors, non-stoichiometric dopants are typically necessary to achieve a high transition temperature, while both structural and chemical defects are used to pin vortices and increase critical current. Scanning tunneling microscopy (STM) has proven to be an ideal technique for studying these processes at the atomic scale. In this perspective, we present an overview of STM studies on chemical disorder in unconventional superconductors, and discuss how dopants, impurities and adatoms may be used to probe, pin or enhance the intrinsic electronic properties of these materials.Physic

Nanoscale visualization of the thermally-driven evolution of antiferromagnetic domains in FeTe thin films

Antiferromagnetic order, being a ground state of a number of exotic quantum materials, is of immense interest both from the fundamental physics perspective and for driving potential technological applications. For a complete understanding of antiferromagnetism in materials, nanoscale visualization of antiferromagnetic domains, domain walls and their robustness to external perturbations is highly desirable. Here, we synthesize antiferromagnetic FeTe thin films using molecular beam epitaxy. We visualize local antiferromagnetic ordering and domain formation using spin-polarized scanning tunneling microscopy. From the atomically-resolved scanning tunneling microscopy topographs, we calculate local structural distortions to find a high correlation with the distribution of the antiferromagnetic order. This is consistent with the monoclinic structure in the antiferromagnetic state. Interestingly, we observe a substantial domain wall change by small temperature variations, unexpected for the low temperature changes used compared to the much higher antiferromagnetic ordering temperature of FeTe. This is in contrast to electronic nematic domains in the cousin FeSe multilayer films, where we find no electronic or structural change within the same temperature range. Our experiments provide the first atomic-scale imaging of perturbation-driven magnetic domain evolution simultaneous with the ensuing structural response of the system. The results reveal surprising thermally-driven modulations of antiferromagnetic domains in FeTe thin films well below the Neel temperature

Emergence of unidirectional coherent quasiparticles from high-temperature rotational symmetry broken phase of AV3Sb5 kagome superconductors

Kagome metals AV3Sb5 display a rich phase diagram of correlated electron states, including superconductivity and novel density waves. Within this landscape, recent experiments reveal signs of a new transition below T ~ 35 K attributed to the highly sought-after electronic nematic phase that spontaneously breaks rotational symmetry of the lattice. We use spectroscopic-imaging scanning tunneling microscopy to study atomic-scale signatures of electronic symmetry breaking as a function of temperature across several materials in this family: CsV3Sb5, KV3Sb5 and Sn-doped CsV3Sb5. We find that rotational symmetry breaking onsets universally at a high temperature in these materials, toward the 2 x 2 charge density wave (CDW) transition temperature T*. At a significantly lower temperature of about 30 K, we discover a striking emergence of the quantum interference of coherent quasiparticles, a key signature for the formation of a coherent electronic state. These quasiparticles display a pronounced unidirectional reciprocal-space fingerprint, which strengthens on approaching the superconducting state. Our experiments reveal that the high-temperature charge ordering states are separated from the superconducting ground state by an intermediate-temperature regime with coherent unidirectional quasiparticles. Their emergence that occurs significantly below the onset of rotational symmetry breaking is phenomenologically different compared to high-temperature superconductors, shedding light on the complex nature of electronic nematicity in AV3Sb5 kagome superconductors

Nanoscale surface element identification and dopant homogeneity in the high-TcT_{c} superconductor PrxCa1−xFe2As2Pr_xCa_{1−x}Fe_2As_2

We use scanning tunneling microscopy to determine the surface structure and dopant distribution in $Pr_xCa_{1−x}Fe_2As_2$, the highest-Tc member of the 122 family of iron-based superconductors. We identify the cleaved surface termination by mapping the local tunneling barrier height, related to the work function. We image the individual Pr dopants responsible for superconductivity, and show that they do not cluster, but in fact repel each other at short length scales. We therefore suggest that the low volume fraction high-Tc superconducting phase is unlikely to originate from Pr inhomogeneity.Physic