Skip to main content

Research Repository

Advanced Search

Exploring the Impact of the HOMO–LUMO Gap on Molecular Thermoelectric Properties: A Comparative Study of Conjugated Aromatic, Quinoidal, and Donor–Acceptor Core Systems

Blankevoort, Nickel; Bastante, Pablo; Davidson, Ross J.; Salthouse, Rebecca J.; Daaoub, Abdalghani H. S.; Cea, Pilar; Solans, Santiago Martin; Batsanov, Andrei S.; Sangtarash, Sara; Bryce, Martin R.; Agrait, Nicolas; Sadeghi, Hatef

Exploring the Impact of the HOMO–LUMO Gap on Molecular Thermoelectric Properties: A Comparative Study of Conjugated Aromatic, Quinoidal, and Donor–Acceptor Core Systems Thumbnail


Authors

Nickel Blankevoort

Pablo Bastante

Ross J. Davidson

Abdalghani H. S. Daaoub

Pilar Cea

Santiago Martin Solans

Sara Sangtarash

Nicolas Agrait

Hatef Sadeghi



Abstract

Thermoelectric materials have garnered significant interest for their potential to efficiently convert waste heat into electrical energy at room temperature without moving parts or harmful emissions. This study investigated the impact of the HOMO–LUMO (H-L) gap on the thermoelectric properties of three distinct classes of organic compounds: conjugated aromatics (isoindigos (IIGs)), quinoidal molecules (benzodipyrrolidones (BDPs)), and donor–acceptor systems (bis­(pyrrol-2-yl)­squaraines (BPSs)). These compounds were chosen for their structural simplicity and linear π-conjugated conductance paths, which promote high electrical conductance and minimize complications from quantum interference. Single-molecule thermoelectric measurements revealed that despite their low H-L gaps, the Seebeck coefficients of these compounds remain low. The alignment of the frontier orbitals relative to the Fermi energy was found to play a crucial role in determining the Seebeck coefficients, as exemplified by the BDP compounds. Theoretical calculations support these findings and suggest that anchor group selection could further enhance the thermoelectric behavior of these types of molecules.

Citation

Blankevoort, N., Bastante, P., Davidson, R. J., Salthouse, R. J., Daaoub, A. H. S., Cea, P., …Sadeghi, H. (2024). Exploring the Impact of the HOMO–LUMO Gap on Molecular Thermoelectric Properties: A Comparative Study of Conjugated Aromatic, Quinoidal, and Donor–Acceptor Core Systems. ACS Omega, 9(7), 8471-8477. https://doi.org/10.1021/acsomega.3c09760

Journal Article Type Article
Acceptance Date Jan 29, 2024
Online Publication Date Feb 5, 2024
Publication Date Feb 20, 2024
Deposit Date Apr 5, 2024
Publicly Available Date Apr 5, 2024
Journal ACS Omega
Publisher American Chemical Society
Peer Reviewed Peer Reviewed
Volume 9
Issue 7
Pages 8471-8477
DOI https://doi.org/10.1021/acsomega.3c09760
Public URL https://durham-repository.worktribe.com/output/2275977

Files




You might also like



Downloadable Citations