Dynamically reconfigurable electronic and phononic properties in intercalated HfS2

Abstract: Dynamic reconfigurability of material properties is essential to enabling innovative neuromorphic- and quantum-computing paradigms. The unique structure of van der Waals layers can facilitate a robust mechanism for this desired reconfigurability. Here, we present a highly versatile and effective approach, based on electrochemical intercalation of organometallics, to control the electron and phonon behavior in hafnium disulfide. Computational and experimental exploration of the physical properties in the intercalated material indicates a significant and measured change. Furthermore, the weak chemical interactions between the organometallics and hafnium disulfide enable an electric-field mediated intercalant drift and charge–discharge process. The control of organometallic concentration in this way provides a dynamic 400-fold control of cross-plane electrical conductivity (1.8?μS/cm–741?μS/cm) and a corresponding 4-fold control of cross-plane thermal conductivity in hafnium disulfide (0.35?Wm−1?K−1–1.45?Wm−1?K−1). Our findings unveil a broad approach to dynamically design layered-material properties for high-performance electronic and phononic applications.