Discovery of a topological exciton insulator with tunable momentum order

Correlated topological materials often maintain a delicate balance among physical symmetries: many topological orders are symmetry protected, while most correlated phenomena arise from spontaneous symmetry breaking. It is rare to find cases where symmetry breaking induces a non-trivial topological phase. Here, we present the discovery of such a phase in Ta2Pd3Te5, where Coulomb interactions form excitons, which condense below 100 K, opening a topological gap and creating a topological excitonic insulator. Our spectroscopy reveals the full spectral bulk gap stemming from exciton condensation. This excitonic insulator state spontaneously breaks mirror symmetries but involves a very weak structural coupling, as indicated by photoemission spectroscopy, thermodynamic measurements, and a detailed structural analysis. Notably, scanning tunneling microscopy uncovers gapless boundary modes in the bulk insulating phase. Their magnetic field response, together with theoretical modeling, suggests a topological origin. These observations establish Ta2Pd3Te5 as the first confirmed topological excitonic insulator in a three-dimensional crystal. This allows to access the associated physics through bulk-sensitive techniques. Furthermore, we uncover another surprising aspect of the topological excitonic insulator, a secondary excitonic instability near 5 K that breaks the translational symmetry. The wavevector of this state shows an unprecedented magnetic field tunability. Thus, we unveil a unique sequence of topological exciton condensations in a bulk crystal, offering new opportunities to study critical behavior and excitations.