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The phenomenon originating from spin-orbit coupling (SOC) providesenergy-efficient strategies for spin manipulation and device applications. Thebroken inversion symmetry interface and resulting electric field induce aRashba-type spin-orbit field (SOF), which has been demonstrated to generatespin-orbit torque for data storage applications. In this study, we found thatspin flipping can be achieved by the valley-Zeeman SOF in monolayer WSe2 atroom temperature, which manifests as a negative magnetoresistance in thevertical spin valve. Quantum transmission calculations based on an effectivemodel near the K valley of WSe2 confirm the precessional spin transport ofcarriers under the giant SOF, which is estimated to be 650 T. In particular,the valley-Zeeman SOF-induced spin dynamics was demonstrated to be tunable withthe layer number and stacking phase of WSe2 as well as the gate voltage, whichprovides a novel strategy for spin manipulation and can benefit the developmentof ultralow-power spintronic devices.

Spin Manipulation by Giant Valley-Zeeman Spin-Orbit Field in Atom-Thick WSe2