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Topological materials hold immense promise for exhibiting exotic quantum phenomena, yet achieving controllable topological phase transitions remains challenging. Here, we demonstrate a structurally driven, reversible topological phase transition in the distorted square net material GdPS, induced via in situ potassium dosing. Using angle-resolved photoemission spectroscopy and first principles calculations, we demonstrate a cascade of topological phases in the subsurface P layer: from a large, topologically trivial band gap to a gapless Dirac cone state with a 2 eV dispersion, and finally to a two-dimensional topological insulator as inferred from theory. This evolution is driven by subtle structural distortions in the first P layer caused by potassium adsorption, which in turn contribute to the band gap closure and topological phase transition. Furthermore, the ability to manipulate the topology of a subsurface layer in GdPS offers a unique route for exploring and controlling topological states in bulk materials. 

Abstract Magnetotransport, the response of electrical conduction to external magnetic field, acts as an important tool to reveal fundamental concepts behind exotic phenomena and plays a key role in enabling spintronic applications. Magnetotransport is generally sensitive to magnetic field orientations. In contrast, efficient and isotropic modulation of electronic transport, which is useful in technology applications such as omnidirectional sensing, is rarely seen, especially for pristine crystals. Here a strategy is proposed to realize extremely strong modulation of electron conduction by magnetic field which is independent of field direction. GdPS, a layered antiferromagnetic semiconductor with resistivity anisotropies, supports a field‐driven insulator‐to‐metal transition with a paradoxically isotropic gigantic negative magnetoresistance insensitive to magnetic field orientations. This isotropic magnetoresistance originates from the combined effects of a near‐zero spin–orbit coupling of Gd³⁺‐based half‐fillingf‐electron system and the strong on‐sitef–dexchange coupling in Gd atoms. These results not only provide a novel material system with extraordinary magnetotransport that offers a missing block for antiferromagnet‐based ultrafast and efficient spintronic devices, but also demonstrate the key ingredients for designing magnetic materials with desired transport properties for advanced functionalities.