Intrinsic Charge Modulation Protocol for Low‐Temperature TMDC Synthesis

ABSTRACT The low‐temperature synthesis of transition metal dichalcogenides (TMDCs) is essential for next‐generation electronics, but this process remains a challenge. Generally, conventional methods require high temperatures, whereas existing low‐temperature approaches depend on extrinsic modifications, such as plasma enhancement or specialized precursors, to enhance reactivity. In this study, a novel fundamental strategy was introduced on the basis of the intrinsic electronic engineering of transition metals (TMs). A bilayered junction protocol was proposed, where a buffer TM (b‐TM) is placed beneath the target TM (t‐TM) to facilitate TMDC synthesis. This junction precisely controls interfacial charge transfer, directly modulating the density of states (DOS) at the Fermi level of t‐TM. The choice of b‐TM enables the bidirectional tuning of DOS at the Fermi level of t‐TM, thereby influencing chalcogen precursor adsorption and systematically reducing the required synthesis temperature. Using this approach, uniform, large‐area TMDC nanosheets (exceeding 5.5 inches) were synthesized at remarkably low temperatures even on glass substrates, demonstrating the method's broad applicability. We have also demonstrated this capability with various TMDCs, including MoS 2 , WS 2 , MoSe 2 , and WSe 2 . Notably, all 25 fabricated memristor arrays on these films demonstrated exceptional performance, achieving remarkably uniform and ultra‐low Set/Reset voltage profiles (±0.15 V). This work establishes a new paradigm for low‐temperature synthesis of TMDCs, potentially applicable to the entire class of TMDCs, paving the way for advanced electronic applications on flexible and transparent substrates.