Dehydrogenation-induced polarity flipping of charge carriers and conductance enhancement in nitrogen-containing heterocyclic molecule-anchored single-molecule junctions

doi:10.1088/1674-1056/ae0d56

Abstract Achieving high conductance and dual charge carriers in molecular junctions is essential for developing logical building blocks in molecular electronics. In this study, we investigated the electrical transport properties of nitrogen-containing heterocyclic molecule (N3C)-anchored single-molecule junctions using the nonequilibrium Green's function based on density functional theory. Our findings reveal that dehydrogenation is an effective strategy for achieving two charge-carrier polarities and improving conductance. In particular, dehydrogenation changed the N3C anchor from an electron-rich to an electron-deficient state, reversing the direction of charge transfer and that of the associated interfacial dipole. Consequently, electrons were replaced by holes as the primary charge carriers. Additionally, the number of removed hydrogen atoms critically governs the charge-transport behavior of molecular junctions. When the anchor groups were connected by conjugated molecular bridges, p-type and n-type molecular junctions were produced by removing three and four hydrogen atoms, respectively, significantly increasing junction conductance in both cases. These findings demonstrate that nitrogen-containing heterocyclic molecules are promising anchor groups for achieving two charge-carrier polarities and enhancing conductance through dehydrogenation.

Keywords: molecular electronics single-molecule devices charge carrier polarity dehydrogenation

Received: 08 July 2025
Revised: 12 September 2025
Accepted manuscript online: 30 September 2025

PACS:	73.63.-b	(Electronic transport in nanoscale materials and structures)
	31.15.at	(Molecule transport characteristics; molecular dynamics; electronic structure of polymers)
	31.15.A-	(Ab initio calculations)
	31.15.E	(Density-functional theory)

Fund: Project supported by the National Natural Science Foundation of China (Grants Nos. 12304316 and 22173052)

Corresponding Authors: Chuan-Kui Wang, Minglang Wang
E-mail: ckwang@sdnu.edu.cn;wangminglang@sdnu.edu.cn

Cite this article:

Qi Zhou(周琦), Ruimei Liu(刘瑞梅), Guang-Ping Zhang(张广平), Chuan-Kui Wang(王传奎), and Minglang Wang(王明郎) Dehydrogenation-induced polarity flipping of charge carriers and conductance enhancement in nitrogen-containing heterocyclic molecule-anchored single-molecule junctions 2026 Chin. Phys. B 35 077301

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Dehydrogenation-induced polarity flipping of charge carriers and conductance enhancement in nitrogen-containing heterocyclic molecule-anchored single-molecule junctions

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