-based van der Waals material*

van der Waals (vdW) materials designed with atomic layers of 2D-based materials exhibit a broad set of novel properties that are highly desirable for enabling heterogeneous device concepts such as neuromorphic and quantum computing. Because of their flexible electronic structure, both carrier dynamics and charge injection are easily tunable with chemical or electrical doping. Using a combined computation and experiment, we demonstrate the feasibility of intercalating electronically active organometallic molecules of two of the family of metallocene: cobaltocene and chromocene into the vdW gap of HfS2-based prototype vdW materials. We achieve high tunability of the electronic and vibrational properties of the hybrid material. Our findings demonstrate a unique approach, leveraging the flexible structural properties of layered materials to create an organic/inorganic interface that tunes and tailor the properties of host materials for distinctive device applications.