Quantum Interference and Contact Effects in Thermoelectric Performance of Anthracene-Based Molecules

TL;DR

This study investigates how different anchor groups and quantum interference affect the electronic and thermoelectric properties of anthracene-based single-molecule junctions, revealing design principles for thermoelectric devices.

Contribution

It provides a comprehensive analysis of contact and interference effects on thermoelectric performance in anthracene molecules, bridging single-molecule and device-level understanding.

Findings

Stronger anchor groups dominate thermoelectric behavior.

Electrode material influences thermopower sign and magnitude.

Transport is consistent with coherent tunneling and Fermi level alignment.

Abstract

We report on the single-molecule electronic and thermoelectric properties of strategically chosen anthracene-based molecules with anchor groups capable of binding to noble metal substrates, such as gold and platinum. Specifically, we study the effect of different anchor groups, as well as quantum interference, on the electric conductance and the thermopower of gold/single-molecule/gold junctions and generally find good agreement between theory and experiment. All molecular junctions display transport characteristics consistent with coherent transport and a Fermi alignment approximately in the middle of the HOMO/LUMO gap. Single-molecule results are in agreement with previously reported thin-film data, further supporting the notion that molecular design considerations may be translated from the single- to the many-molecule devices. For combinations of anchor groups where one binds significantly more strongly to the electrodes than the other, the stronger anchor group appears to dominate the thermoelectric behaviour of the molecular junction. For other combinations, the choice of electrode material can determine the sign and magnitude of the thermopower. This finding has important implications for the design of thermoelectric generator devices, where both n- and p-type conductor are required for thermoelectric current generation.