Searches for permanent electric dipole moments (EDMs) probe new sources of CP violation beyond the Standard Model. The atomic EDM of , which is sensitive to its nuclear Schiff moment, is a promising candidate, but previous measurements were limited by noise and systematic effects induced by the optical dipole trap (ODT) that holds the atoms. Here we report a substantially improved search enabled by a dual-ODT configuration with orthogonal polarizations, and spin measurements for precise alignment of static and optical fields. By suppressing the key parity-mixing systematic effect and vector light-shift noise, we achieve a limit of (95% C.L.), which represents a 20-fold improvement over the previous work. We also present the first calculation of the nuclear structure factors of the Schiff moment of . The experimental and theoretical advances combine to tighten constraints on CP-violating pion-nucleon couplings in a global analysis. Moreover, this work demonstrates a pathway toward future measurements in , where nuclear deformation offers exceptional sensitivity to physics beyond the Standard Model.

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