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Abstract

The infinite-layer compound CaCoO2 provides a compelling platform to explore how local orbital distortions evolve into collective electronic order. Using resonant soft x-ray scattering (RSXS) and its time-resolved counterpart (tr-RSXS), we reveal a cooperative coupling between two intertwined orders at the same in-plane wave vector, q≈(1/4,1/4,0), comprising a quasi-two-dimensional orbital order associated with the distorted Co(1) sites and a quasi-three-dimensional trimerlike charge order stabilized through Co-O-Ca hybridization. The charge-sensitive component exhibits a uniform relaxation time of ∼400 fs (391±5 fs) across multiple Co resonances, evidencing a collective charge response. A comparable timescale observed in the orbital order associated with the highly distorted Co(1) sites indicates that this collective behavior naturally originates from the same orbital framework that mediates both charge and orbital degrees of freedom. Together, these findings establish CaCoO2 as a model system in which Jahn-Teller distortions, orbital hybridization, and geometric frustration cooperate to form molecular trimer units that dictate the macroscopic electronic behavior.

Document Type

Article

Publication Date

1-1-2026

Notes/Citation Information

Publisher Copyright: © 2026 authors. Published by the American Physical Society.

Digital Object Identifier (DOI)

10.1103/scdr-tmq4

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