Intercalation of transition metal atoms into layered materials is a powerful method to tune the electronic structure and carrier-transport properties of semiconductor host materials. However, metal atom intercalation into group VI transition metal dichalcogenides (TMDs) including MoS2 and WS2 is challenging because this process is thermodynamically unfavorable. Here, we utilize n-butyllithium to reductively activate WS2 nanosheets and thereby drive the intercalation of vanadium complexes through ion diffusion. The strong interaction between V2/3+ in the interlayer galleries with the WS2 basal planes increases the bulk conductivity by 2 orders of magnitude and decreases the activation energy for carrier transport by 8 times. Moreover, V intercalation converts bulk WS2 from a p-type to an n-type semiconductor based on Hall effect measurements. Kelvin-probe force microscopy confirms the Fermi level has a shift of 60 meV towards the conduction band due to the hybridization of V d-orbitals with the conduction band of WS2. Our work provides a general method for the intercalation of transition metal atoms into Group VI TMDs and provides insight into the electronic interactions and impact carrier transport and conductivity.

Vanadium intercalated WS2 with tunable electronic properties

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