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We propose a possible route to achieve high thermoelectric efficiency inmolecular junctions by combining a local chemical tuning of the molecularelectronic states with the use of semiconducting electrodes. The former allowsto control the position of the HOMO transmission resonance with respect to theFermi energy while the latter fulfills a twofold purpose: the suppression ofelectron-like contributions to the thermopower and the cut-off of the HOMOtransmission tails into the semiconductor band gap. As a result a largethermopower can be obtained. Our results strongly suggest that large figures ofmerit in such molecular junctions can be achieved.

Engineering the thermopower in semiconductor-molecule junctions: towards high thermoelectric efficiency at the nanoscale