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Time-reversal symmetry breaking (TRSB) in magnetic topological insulators induces a Dirac gap in the topological surface state (TSS), leading to exotic phenomena such as the quantum anomalous Hall effect. Yet, the interplay between TRSB and topology in superconductors remains underexplored due to limited suitable materials. Here we employ zero-fieldmuon spin relaxation (μSR) as a sensitive probe of TRSB to map out the electronic phase diagrams of iron-chalcogenide superconductors FeSe1−xTex. For the Te composition x = 0.64 with the highest superconducting transition temperature Tc = 14.5K, which is known to host a TSS and Majorana zero modes within vortices, we detect spontaneous magnetic fields below Tc distinct from a magnetic order. This signifies a TRSB superconducting state in the bulk, revealing the convergence of unconventional TRSB superconductivity with topologically nontrivial electronic structures in FeSe1−xTex. Given the relatively high Tc and the tunability of the Fermi level through chemical substitution, iron-chalcogenide superconductors offer an intriguing platform for investigating the synergy between topological superconductivity and TRSB. 

Abstract Kramers degeneracy is one fundamental embodiment of the quantum mechanical nature of particles with half-integer spin under time reversal symmetry. Under the chiral and noncentrosymmetric achiral crystalline symmetries, Kramers degeneracy emerges respectively as topological quasiparticles of Weyl fermions and Kramers nodal lines (KNLs), anchoring the Berry phase-related physics of electrons. However, an experimental demonstration for ideal KNLs well isolated at the Fermi level is lacking. Here, we establish a class of noncentrosymmetric achiral intercalated transition metal dichalcogenide superconductors with large Ising-type spin-orbit coupling, represented by In_xTaS₂, to host an ideal KNL phase. We provide evidence from angle-resolved photoemission spectroscopy with spin resolution, angle-dependent quantum oscillation measurements, and ab-initio calculations. Our work not only provides a realistic platform for realizing and tuning KNLs in layered materials, but also paves the way for exploring the interplay between KNLs and superconductivity, as well as applications pertaining to spintronics, valleytronics, and nonlinear transport. 

Dataset for publication "Kramers nodal lines in intercalated TaS2 superconductors". Detailed descriptions are in the README text documents in subdirectories.