Intrinsic Ultrafast Edge Photocurrent Dynamics in WTe₂Driven by Broken Crystal Symmetry

Directional photocurrents in two-dimensional materials arise from broken crystal symmetry, offering pathways to high-speed, bias-free photodetection beyond conventional devices. Tungsten ditelluride (WTe₂), a type-II Weyl semimetal, exhibits robust symmetry-breaking-induced edge photocurrents from competing nonlinear optical and photothermoelectric mechanisms, whose intrinsic dynamics have remained experimentally inaccessible. Here, we directly resolve subpicosecond edge photocurrent dynamics in WTe₂ through ohmic contacts over temperatures from 300 to 4 K. We demonstrate ultrafast optical-to-electrical conversion with a 3 dB bandwidth of ∼250 GHz and reveal picosecond-timescale switching of the net photocurrent direction below 150 K, linked to a Lifshitz transition. This transient bipolar response arises from nonequilibrium Seebeck effects due to asymmetric cooling of hot electrons and holes. These findings reveal previously hidden ultrafast dynamics in symmetry-engineered materials, offering new strategies to disentangle competing photocurrent mechanisms and enabling the development of self-powered, ultrafast optoelectronic devices.