Giant unusual anisotropic magnetoresistance enabled by hole-electron resonance in van der Waals heterostructures.

The hole-electron resonance in two-dimensional WTe2 dynamically screens the built-in electric field, disrupting the scattering equilibrium constraints of conventional electron transport. Here, we propose utilizing the hole-electron resonance to achieve Coulomb force-unconstrained spin angular momentum transfer across the WTe2/Fe3GaTe2 interface, offering a novel platform for exploring unconventional spin transport phenomena. A clear signature of this mechanism is the observation of an unusual anisotropic magnetoresistance of 289%, which far exceeds conventional spin Hall magnetoresistance and cannot be explained by standard spin absorption or scattering models. Its angular profile deviates from the simple cosine-squared form but realigns after accounting for magnetization and field orientation, reflecting the interplay between hole-electron resonance and magnetization dynamics. Furthermore, chiral transverse transport with distinct symmetry transitions emerges within the hole-active temperature regime, originating from interfacial symmetry breaking and the inhomogeneous spin-orbital coupling. These findings highlight the essential roles of both electrons and holes in spin transport.