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Prior ultralow thermal conductivity materials are not suitable forthermoelectric applications due to the limited electronic transport in thematerials. Here, we present a new class of ultralow thermal conductivitymaterials with substantial electronic heat transport. Our samples aregraphene/metal heterostructures of transferred graphene and ultrathin metalfilms (Pd, Au and Ni) deposited by either thermal evaporation or rf magnetronsputtering. For the evaporated samples, we achieve an ultralow thermalconductivity of 0.06 W m-1 K-1, with phonons as the dominant heat carriers. Theultralow thermal conductivity is due to a huge disparity in phonon energy ingraphene and metals. Interestingly, for the sputtered samples, we find thatabout 50 % of heat is carried by electrons, even when thermal conductivity isabout 0.1 W m-1 K-1. We attribute the electronic contribution to transmissionof electrons across atomic-scale pinholes in graphene. With the ultralowthermal conductivity and substantial electronic transport, the new materialscould be explored for thermoelectric applications.

Tuning electronic heat transport in graphene/metal heterostructures with ultralow thermal conductivity