Exploring Aromaticity Effects on Electronic Transport in Cyclo[n]carbon Single-Molecule Junctions

Overview

Journal Molecules

Publisher MDPI

Specialty Biology

Date 2024 Aug 29

PMID 39202906

Authors

Peiqi Yang

Haoyang Pan

Yudi Wang

Jie Li

Yangyu Dong

Yongfeng Wang

Shimin Hou

Affiliations

Soon will be listed here.

Abstract

Cyclo[n]carbon (C) is one member of the all-carbon allotrope family with potential applications in next-generation electronic devices. By employing first-principles quantum transport calculations, we have investigated the electronic transport properties of single-molecule junctions of C, with n = 14, 16, 18, and 20, connected to two bulk gold electrodes, uncovering notable distinctions arising from the varying aromaticities. For the doubly aromatic C and C molecules, slightly deformed complexes at the singlet state arise after bonding with one Au atom at each side; in contrast, the reduced energy gaps between the highest occupied and the lowest unoccupied molecular orbitals due to the orbital reordering observed in the doubly anti-aromatic C and C molecules lead to heavily deformed asymmetric complexes at the triplet state. Consequently, spin-unpolarized transmission functions are obtained for the Au-C-Au junctions, while spin-polarized transmission appears in the Au-C-Au junctions. Furthermore, the asymmetric in-plane π-type hybrid molecular orbitals of the Au-C-Au junctions contribute to two broad but low transmission peaks far away from the Fermi level (), while the out-of-plane π-type hybrid molecular orbitals dominate two sharp transmission peaks that are adjacent to , thus resulting in much lower transmission coefficients at compared to those of the Au-C-Au junctions. Our findings are helpful for the design and application of future cyclo[n]carbon-based molecular electronic devices.

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