Thickness-Dependent Spintronic Terahertz Emission in MBE-Grown PtTe$_2$: From Semiconductor to Type-II Dirac Semimetal
Spintronic terahertz (THz) emitters have established themselves as among the most practical broadband THz sources available, yet their performance remains fundamentally limited by the spin Hall conductivity of the nonmagnetic conversion layer - a quantity that is fixed once the material is chosen. Here, we demonstrate that in PtTe$_2$, a type-II Dirac semimetal within the transition metal dichalcogenide family, this limitation can be circumvented by exploiting the dramatic thickness-driven electronic phase evolution of the material itself. Using molecular beam epitaxy to grow PtTe$_2$ films with single-monolayer precision from 1 to 20 ML, we show that the spintronic THz emission tracks the underlying electronic phase diagram directly: it is absent in the single-layer semiconducting phase, turns on sharply at the semimetal transition near 2 ML, and reaches a peak amplitude six times that of an equivalent Pt reference at 10 ML, before declining at larger thicknesses due to THz reabsorption in the increasingly metallic film. This non-monotonic behavior is inconsistent with a bulk inverse spin Hall mechanism and instead reflects a multi-channel spin-to-charge conversion process in which spin-momentum-locked topological surface states and a thickness-dependent interfacial Rashba splitting both contribute and strengthen as the type-II Dirac band structure develops. First-principles calculations of the interfacial spin accumulation reproduce the experimental trend quantitatively, confirming this physical picture. These findings introduce thickness engineering of van der Waals semimetals as a new and accessible route to optimizing spintronic THz emitters and spin-orbit torques in magnetic memories (SOT-MRAMs), with direct implications for the broader class of dimensionally tunable topological materials.