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Giant thermoelectric effect in graphene-based topological insulators with heavy adatoms and nanopores.

Designing thermoelectric materials with high figure of merit ZT = S(2)GT/Ktot requires fulfilling three often irreconcilable conditions, that is, the high electrical conductance G, small thermal conductance Ktot, and high Seebeck coefficient S. Nanostructuring is one of the promising ways to achieve this goal as it can substantially suppress lattice contribution to Ktot. However, it may also unfavorably influence the electronic transport in an uncontrollable way. Here, we theoretically demonstrate that this issue can be ideally solved by fabricating graphene nanoribbons with heavy adatoms and nanopores. The adatoms locally enhance spin-orbit coupling in graphene thereby converting it into a two-dimensional topological insulator with a band gap in the bulk and robust helical edge states, which carry electrical current and generate a highly optimized power factor S(2)G per helical conducting channel due to narrow boxcar-function-shaped electronic transmission (surpassing even the Mahan-Sofo limit obtained for delta-function-shaped electronic transmission). Concurrently, the array of nanopores impedes the lattice thermal conduction through the bulk. Using quantum transport simulations coupled with first-principles electronic and phononic band structure calculations, the thermoelectric figure of merit is found to reach its maximum ZT ≃ 3 at low temperatures T ≃ 40 K. This paves a way to design high-ZT materials by exploiting the nontrivial topology of electronic states through nanostructuring.