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Two-dimensional (2D) topological insulators (TIs) with a large bulk band-gapare promising for experimental studies of the quantum spin Hall effect and forspintronic device applications. Despite considerable theoretical efforts inpredicting large-gap 2D TI candidates, only few of them have beenexperimentally verified. Here, by combining scanning tunnelingmicroscopy/spectroscopy and angle-resolved photoemission spectroscopy, wereveal that the top monolayer of ZrTe5 crystals hosts a large band gap of ~100meV on the surface and a finite constant density-of-states within the gap atthe step edge. Our first-principles calculations confirm the topologicallynontrivial nature of the edge states. These results demonstrate that the topmonolayer of ZrTe5 crystals is a large-gap 2D TI suitable for topotronicapplications at high temperature.

Experimental evidence of large-gap two-dimensional topological insulator on the surface of ZrTe5