Simultaneous description of conductance and thermopower in single-molecule junctions from many-body ab initio calculations

Chengjun Jin, Troels Markussen, Kristian Sommer Thygesen

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We investigate the electronic conductance and thermopower of a single-molecule junction consisting of bis-(4-aminophenyl) acetylene (B4APA) connected to gold electrodes. We use nonequilibrium Green's function methods in combination with density-functional theory (DFT) and the many-body GW approximation. To simulate recent break junction experiments, we calculate the transport properties of the junction as it is pulled apart. For all junction configurations, DFT with a standard semilocal functional overestimates the conductance by almost an order of magnitude, while the thermopower is underestimated by up to a factor of 3, except for the most highly stretched junction configurations. In contrast, the GW results for both conductance and thermopower are in excellent agreement with experiments for a wide range of electrode separations. We show that the GW self-energy not only renormalizes the molecular energy levels but also the coupling strength. The latter is a consequence of the finite response time associated with the electronic screening in the metal electrodes.
Original languageEnglish
JournalPhysical Review B
Issue number7
Pages (from-to)075115
Number of pages8
Publication statusPublished - 2014

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©2014 American Physical Society

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