Modulation of Spin Dynamics in 2D Transition‐Metal Dichalcogenide via Strain‐Driven Symmetry Breaking

Transition metal dichalcogenides (TMDs) possess intrinsic spin–orbit interaction (SOI) with high potential to be exploited for various quantum phenomena. SOI allows the manipulation of spin degree of freedom by controlling the carrier's orbital motion via mechanical strain. Here, strain modulated spin dynamics in bilayer MoS(2) field‐effect transistors (FETs) fabricated on crested substrates are demonstrated. Weak antilocalization (WAL) is observed at moderate carrier concentrations, indicating additional spin relaxation path caused by strain fields arising from substrate crests. The spin lifetime is found to be inversely proportional to the momentum relaxation time, which follows the Dyakonov–Perel spin relaxation mechanism. Moreover, the spin–orbit splitting is obtained as 37.5 ± 1.4 meV, an order of magnitude larger than the theoretical prediction for monolayer MoS(2), suggesting the strain enhanced spin‐lattice coupling. The work demonstrates strain engineering as a promising approach to manipulate spin degree of freedom toward new functional quantum devices.