Abstract
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-field muon spin relaxation (μSR) as a sensitive probe of TRSB to map out the electronic phase diagrams of iron-chalcogenide superconductors FeSe(1-x)Te(x). For the Te composition x = 0.64 with the highest superconducting transition temperature T(c) = 14.5 K, which is known to host a TSS and Majorana zero modes within vortices, we detect spontaneous magnetic fields below T(c) 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 FeSe(1-x)Te(x). Given the relatively high T(c) 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.