Topological phases of matter have established a new paradigm in physics, bringing quantum phenomena to the macroscopic scale and hosting exotic emergent quasiparticles. In this thesis, I theoretically and experimentally demonstrate with my collaborators the first Weyl semimetal, TaAs, using angle-resolved photoemission spectroscopy (ARPES), directly observing its emergent Weyl fermions and topological Fermi arc surface states [Science 349, 6248 (2015); Nat. Commun. 6, 7373 (2015); PRL 116, 066802 (2016)]. Next, I discover high-degeneracy topological chiral fermions in the chiral crystals RhSi and CoSi, with wide topological energy window, maximal separation in momentum space and giant Fermi arcs [Nature 567, 500 (2019); Nat. Mat. 17, 978 (2018)]. I establish a natural relationship between the structural and topological chirality, associated with a robust topological state which we predict supports a four-unit quantized photogalvanic effect [PRL 119, 206401 (2017)]. I also discuss the first quantum topological superlattice, in multilayer heterostructures consisting of alternating topological and trivial insulators [Sci. Adv. 3, e1501692 (2017)]. The Dirac cones at each interface tunnel across layers, forming an emergent atomic chain where the Dirac cones serve as atomic orbitals. I achieve unprecedented control of hopping amplitudes within the superlattice, realizing a topological phase transition. Lastly, I discover a room-temperature topological magnet in Co$_2$MnGa [Science 365, 1278 (2019); PRL 119, 156401 (2017)]. I observe topological Weyl lines and drumhead surface states by ARPES, demonstrating a topological invariant supported by the materials intrinsic magnetic order. I also find that the large anomalous Hall effect in Co$_2$MnGa arises from the Weyl lines. I hope that my discovery of Co$_2$MnGa establishes topological magnetism as a new frontier in condensed matter physics.
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