<p>Interconnecting the surfaces of nanomaterials
without compromising their outstanding mechanical, thermal, and electronic
properties is critical in the design of advanced bulk structures that still preserve
the novel properties of their nanoscale constituents. As such, bridging the p-conjugated carbon
surfaces of single-walled carbon nanotubes (SWNTs) has special implications in
next-generation electronics. This study presents a rational path towards
improvement of the electrical transport in aligned semiconducting SWNT films by
deposition of metal atoms. The formation of conducting Cr-mediated pathways
between the parallel SWNTs increases the transverse (intertube) conductance,
while having negligible effect on the parallel (intratube) transport. In
contrast, doping with Li has a predominant effect on the intratube electrical
transport of aligned SWNT films. Large-scale first-principles calculations of
electrical transport on aligned SWNTs show good agreement with the experimental
electrical measurements and provide insight into the changes that different
metal atoms exert on the density of states near the Fermi level of the SWNTs
and the formation of transport channels. </p>