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Large area van der Waals (vdW) thin films are assembled materials consistingof a network of randomly stacked nanosheets. The multi-scale structure and thetwo-dimensional nature of the building block mean that interfaces naturallyplay a crucial role in the charge transport of such thin films. While single orfew stacked nanosheets (i.e. vdW heterostructures) have been the subject ofintensive works, little is known about how charges travel through multilayered,more disordered networks. Here we report a comprehensive study of aprototypical system given by networks of randomly stacked reduced grapheneoxide 2D nanosheets, whose chemical and geometrical properties can becontrolled independently, permitting to explore percolated networks rangingfrom a single nanosheet to some billions with room temperature resistivityspanning from 10-5 to 10-1 ohm m. We systematically observe a clear transitionbetween two different regimes at a critical temperature T*: Efros-Shklovskiivariable range hopping (ESVRH) below T* and power law (PL) behavior above.Firstly, we demonstrate that the two regimes are strongly correlated with eachother, both depending on the charge localization length xi, calculated byES-VRH model, which corresponds to the characteristic size of overlapping sp2domains belonging to different nanosheets. Thus, we propose a microscopic modeldescribing the charge transport as a geometrical phase transition, given by themetal-insulator transition associated with the percolation of quasi-1Dnanofillers with length xi, showing that the charge transport behavior of thenetworks is valid for all geometries and defects of the nanosheets, ultimatelysuggesting a generalized description on vdW and disordered thin films.

Multiscale charge transport in van der Waals thin films: reduced graphene oxide as case study