Interface Engineering of Chemical Vapor‐Deposited 2D MoSe₂

The drive to harness 2D materials in next‐generation electronics and optoelectronics hinges on precise control over their fundamental properties. Among the diverse 2D systems, transition metal dichalcogenides (TMDs), such as MoS 2 and MoSe 2 , exhibit tunable bandgaps and outstanding carrier mobilities, making them prime candidates for miniaturized devices. Here, two interface engineering approaches are employed—surface fluorination by XeF 2 exposure and nitrogen implantation via low‐energy N + ion beams—to systematically probe how atomic‐level modifications affect chemical vapor‐deposited MoSe 2 . Raman and X‐ray photoelectron spectroscopies reveal that the fluorination induces subtle crystal‐lattice changes with partial fluorine incorporation, forming FMo and FO bonds and inducing mild p‐type doping. In contrast, the nitrogen implantation leads to more pronounced structural alterations, including increased defect density and MoN bond formation, resulting in marked n‐type doping. These findings underscore the versatility of combining fluorination and nitrogen implantation to tailor 2D TMDs, offering new avenues for designing advanced optoelectronic and electronic devices with precisely engineered functionalities.