Observation of Iso-Symmetric Structural and Lifshitz Transitions in Quasi-One-Dimensional CrNbSe₅

Chalcogenides-rich transition metal compounds host a rich landscape of emergent quantum phenomena that are intimately governed by their quasi-one-dimensional chemical-bonding frameworks and their response to external perturbations such as pressure. Here, we report a pressure-induced iso-symmetric structural transition in the quasi-one-dimensional compound CrNbSe₅, in which the electronic ground state is controlled not by symmetry breaking but by a continuous reorganization of local bonding interactions. Applied pressure reversibly tunes CrNbSe₅ between semiconducting and semimetallic states, enabling access to low- and high-carrier electronic regimes through direct modulation of metal-chalcogen bonding. High-pressure single-crystal X-ray diffraction directly resolves the evolution of Cr-Se and Nb-Se bond distances, coordination polyhedra, and connectivity, revealing a fully reversible semimetal-semiconductor-semimetal transition driven by gradual yet cooperative bond rearrangements within a preserved crystallographic symmetry. In contrast to chemical substitution, which irreversibly alters composition and introduces disorder, pressure acts as a clean, continuous control parameter that reshapes the bonding landscape without disrupting structural symmetry. These results establish CrNbSe₅ as a model system for electronically driven phase switching via tunable chemical bonding, highlighting iso-symmetric bond reorganization as a powerful design principle for pressure-controlled electronic and spintronic functionalities.