We carried out systematic neutron scattering experiments to investigate the magnetic properties and their relationship to the high-$T_c$ superconductivity, when the materials are tuned from their antiferromagnetic (AF) parent compounds to the superconducting regime. We observed resonance mode in the electron doped cuprate Nd$_{1.85}$Ce$_{0.15}$CuO$_4$, demonstrating that the resonance is a general phenomenon in cuprate superconductors regardless of hole- or electron-doping. In Pr$_{0.88}$LaCe$_{0.12}$CuO$_4$, the local susceptibility displays two distinct energy scales that are broadly consistent with the bosonic modes revealed by scanning tunneling microscopy experiments. These results indicate the presence of very strong electron spin excitations couplings in electron doped cuprates. Shortly after the discovery of high-$T_c$ superconductivity in the Fe pnictides, we discovered that the magnetic phase diagram of CeFeAsO$_{1-x}$F$_x$ is remarkably similar to that of the cuprates. Besides CeFeAsO, similar magnetic and lattice structures are also observed in PrFeAsO and SrFe$_2$As$_2$ systems. Neutron scattering measurements show that in SrFe$_2$As$_2$, the spectrum of magnetic excitations consists of a Bragg peak at the elastic position, a spin gap, and sharp spin-wave excitations at higher energies. Based on the observed dispersion relation, we estimated the effective magnetic exchange coupling using a Heisenberg model. In order to study the nature of the exchange interactions in the parent compound of Fe pnictides, we studied the high energy spin-wave excitations in CaFe$_2$As$_2$. Although the spin waves in the entire Brillouin zone can be described by an effective three-dimensional anisotropic Heisenberg Hamiltonian, the magnetism in this system is neither purely local nor purely itinerant; rather it is a complicated mix of the two. When the Fe pnictide is tuned into superconducting regime with doping, the low energy spin fluctuation is dominated by a resonance mode. In the optimally electron doped BaFe$_{1.9}$Ni$_{0.1}$As$_2$, application of a magnetic field that suppresses the superconductivity and superconducting gap energy also reduces the intensity and energy of the resonance. These results suggest that the energy of the resonance is proportional to the electron pairing energy, and thus indicate that spin fluctuations are intimately related to the mechanism of high $T_c$ superconductivity.

Thesis advisor: Ilija Zeljkovic / The splendid world of quantum materials is being unveiled in modern condensed matter physics, thanks to the advanced material synthesis methods, refined experimental probing techniques and deeper theoretical understanding. Unconventional superconductivity and topological phenomena are two of the main themes in this realm. Many outstanding problems are waiting to be solved and there is also a great potential in future technological applications. Among many routes of studying the quantum materials, creating thin film structures provides a special opportunity to learn the physical properties in low dimensions, to explore the effect of substrate and strain and to make novel electronic devices.In this thesis, I will present successful molecular beam epitaxy thin film synthesis of: (1) unconventional superconductor FeSe, (2) topological insulator Bi2Se3 doped with magnetic Fe atoms and (3) kagome structure magnets FeSn and Fe3Sn2. For (1), I will describe the finding of a dislocation network, its impact on the spatially-modulated strain field and its interesting interplay with the spontaneous symmetry-broken nematic phase. This is a new finding in the FeSe/SrTiO3 heterostructure and also provides fresh insights in the understandings of nematicity. For (2), I will show how we cross-check the doping ratio using different characterization techniques. Our observation indicates the possible formation of Fe clusters or impurity phases and sets the foundation for future synthesis of similar structures. For (3), I will demonstrate the novel selective synthesis of FexSny thin films. A plethora of spectral features were found in Fe3Sn2, implying a link with the Weyl physics. The FexSny thin films can potentially be a platform for the exploration of correlated, topological quantum phases in low dimensions. / Thesis (PhD) — Boston College, 2022. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Physics.