Thermoelectric Enhancement of Series-Connected Cross-Conjugated Molecular Junctions

TL;DR

This paper explores how series-connected cross-conjugated molecules can enhance thermoelectric performance through quantum effects.

Contribution

The study introduces a new quantum-enhanced thermoelectric mechanism using split-node spectra in series-connected molecular junctions.

Findings

Increasing repeat units in cross-conjugated junctions maintains the fundamental gap but enhances thermopower.

Split-node-based materials outperform interference-based mechanisms like supernode coalescence.

Quantum interference in series-connected architectures improves thermoelectric efficiency and ZT scaling.

Abstract

We investigate the thermoelectric response of single-molecule junctions composed of acyclic cross-conjugated molecules, including dendralene analogues and related iso-poly(diacetylene) (iso-PDA) motifs, in which node-possessing repeat units are connected in series. Using many-body quantum transport theory, we show that increasing the number of repeat units leaves the fundamental gap essentially unchanged while giving rise to a split-node spectrum whose cumulative broadening dramatically enhances the thermopower. This form of quantum enhancement can exceed other interference-based mechanisms, such as the coalescence of nodes into a supernode, suggesting new opportunities for scalable quantum-interference–based materials. Although illustrated here with cross-conjugated systems, the underlying principles apply broadly to series-connected architectures hosting multiple interference nodes. Finally, we evaluate the scaling of the electronic figure of merit ZT and the maximum thermodynamic efficiency. Together, these results highlight the potential for split-node-based materials to realize quantum-enhanced thermoelectric response.

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