Band transport by large Fröhlich polarons in MXenes

Abstract

MXenes are emerging layered materials that are promising for electrochemical energy storage and (opto-)electronic applications. A fundamental understanding of charge transport in MXenes is essential for such applications, but has remained under debate. While theoretical studies pointed to efficient band transport, device measurements have revealed thermally activated, hopping-type transport. Here we present a unifying picture of charge transport in two model MXenes by combining ultrafast terahertz and static electrical transport measurements to distinguish the short- and long-range transport characteristics. We find that band-like transport dominates short-range, intra-flake charge conduction in MXenes, whereas long-range, inter-flake transport occurs through thermally activated hopping, and limits charge percolation across the MXene flakes. Our analysis of the intra-flake charge carrier scattering rate shows that it is dominated by scattering from longitudinal optical phonons with a small coupling constant (α ≈ 1), for both semiconducting and metallic MXenes. This indicates the formation of large polarons in MXenes. Our work therefore provides insight into the polaronic nature of free charges in MXenes, and unveils intra- and inter-flake transport mechanisms in the MXene materials, which are relevant for both fundamental studies and applications.