Quantum interference and heteroaromaticity of para-and meta-linked bridged biphenyl units in single molecular conductance measurements
Markus Gantenbein,Lin Wang,Alaa A. Al-Jobory,Ali K. Ismael,Ali K. Ismael,Colin J. Lambert,Wenjing Hong,Wenjing Hong,Martin R. Bryce +8 more
Reads0
Chats0
TLDR
This study establishes that both quantum interference and heteroaromaticity in the molecular core units play important and inter-related roles in determining the conductance of single molecular junctions.Abstract:
Is there a correlation between the (hetero)aromaticity of the core of a molecule and its conductance in a single molecular junction? To address this question, which is of fundamental interest in molecular electronics, oligo(arylene-ethynylene) (OAE) molecular wires have been synthesized with core units comprising dibenzothiophene, carbazole, dibenzofuran and fluorene. The biphenyl core has been studied for comparison. Two isomeric series have been obtained with 4-ethynylpyridine units linked to the core either at para-para positions (para series 1–5) or meta-meta positions (meta series 6–10). A combined experimental and computational study, using mechanically controlled break junction measurements and density functional theory calculations, demonstrates consistently higher conductance in the para series compared to the meta series: this is in agreement with increased conjugation of the π–system in the para series. Within the para series conductance increases in the order of decreasing heteroaromaticity (dibenzothiophene < carbazole < dibenzofuran). However, the sequence is very different in the meta series, where dibenzothiophene ≈ dibenzofuran < carbazole. Excellent agreement between theoretical and experimental conductance values is obtained. Our study establishes that both quantum interference and heteroaromaticity in the molecular core units play important and inter-related roles in determining the conductance of single molecular junctions.read more
Citations
More filters
Single-Molecule Junctions Based on Nitrile-Terminated Biphenyls
Linda A. Zotti,Artem Mishchenko,David Vonlanthen,Marius Bürkle,Fabian Pauly,Juan Carlos Cuevas,Marcel Mayor,Thomas Wandlowski +7 more
TL;DR: It is found both theoretically and experimentally that the conductance of the molecular junctions is roughly proportional to the square of the cosine of the torsion angle between the two benzene rings of the biphenyl core, which demonstrates the robustness of this structure-conductance relationship.
Journal ArticleDOI
Conductance Switching in Expanded Porphyrins through Aromaticity and Topology Changes
Thijs Stuyver,Mickael L. Perrin,Mickael L. Perrin,Paul Geerlings,Frank De Proft,Mercedes Alonso +5 more
TL;DR: It is shown that expanded porphyrins, upon redox and topology interconversions, could act as efficient three-level molecular switches with high ON/OFF ratio, up to 103 at low bias voltage.
Journal ArticleDOI
Heteroatom-induced molecular asymmetry tunes quantum interference in charge transport through single-molecule junctions.
Yang Yang,Markus Gantenbein,Afaf Alqorashi,Junying Wei,Sara Sangtarash,Duan Hu,Hatef Sadeghi,Rui Zhang,Jiuchan Pi,Li-Chuan Chen,Xiaoyan Huang,Ruihao Li,Junyang Liu,Jia Shi,Wenjing Hong,Colin J. Lambert,Martin R. Bryce +16 more
TL;DR: In this article, the interplay between quantum interference and molecular asymmetry in charge transport through a single molecule was studied, and it was found that the symmetric molecules are more conductive than their asymmetric isomers and that there is no statistically significant dependence on the aromaticity of the core.
Journal ArticleDOI
Charge transfer complexation boosts molecular conductance through Fermi level pinning
Kun Wang,Andrea Vezzoli,Iain Grace,Maeve McLaughlin,Richard J. Nichols,Bingqian Xu,Colin J. Lambert,Simon J. Higgins +7 more
TL;DR: In this paper, a charge transfer complex with tetracyanoethylene (TCNE) was proposed to increase charge transport efficiency in long and poorly conductive molecular wires, with important repercussions in single-entity thermoelectronics and spintronics.
References
More filters
Journal ArticleDOI
The SIESTA method for ab initio order-N materials simulation
José M. Soler,Emilio Artacho,Julian D. Gale,Alberto García,Javier Junquera,Javier Junquera,Pablo Ordejón,Daniel Sánchez-Portal +7 more
TL;DR: In this paper, a selfconsistent density functional method using standard norm-conserving pseudopotentials and a flexible, numerical linear combination of atomic orbitals basis set, which includes multiple-zeta and polarization orbitals, was developed and implemented.
Journal ArticleDOI
Conductance of a Molecular Junction
Mark A. Reed,Mark A. Reed,Chongwu Zhou,Chongwu Zhou,C. J. Muller,C. J. Muller,T. P. Burgin,T. P. Burgin,James M. Tour,James M. Tour +9 more
TL;DR: In this paper, benzene-1,4-dithiol molecules were self-assembled onto the two facing gold electrodes of a mechanically controllable break junction to form a statically stable gold-sulfur-aryl-solfur-gold system, allowing for direct observation of charge transport through the molecules.
Journal ArticleDOI
Measurement of Single-Molecule Resistance by Repeated Formation of Molecular Junctions
Bingqian Xu,Nongjian Tao +1 more
TL;DR: The conductance of a single molecule connected to two gold electrodes was determined by repeatedly forming thousands of gold-molecule-gold junctions using conductance histograms, which revealed well-defined peaks at integer multiples of a fundamental conductance value.
Journal ArticleDOI
Dependence of single-molecule junction conductance on molecular conformation
Latha Venkataraman,Jennifer E. Klare,Colin Nuckolls,Mark S. Hybertsen,Michael L. Steigerwald +4 more
TL;DR: Amine link groups are used to form single-molecule junctions with more reproducible current–voltage characteristics and it is found that the conductance for the series decreases with increasing twist angle, consistent with a cosine-squared relation predicted for transport through π-conjugated biphenyl systems.
Journal ArticleDOI
Exchange-correlation energy of a metallic surface: Wave-vector analysis
David C. Langreth,John P. Perdew +1 more
TL;DR: In this paper, the exchange-correlation energy of a jellium metal surface is analyzed in terms of the wavelength of the fluctuations that contribute to it, using a three-dimensional scheme different from that used by other authors.