@article{e143865711ae49d999237b9b4da25a0b,
title = "Shape-persistent ladder molecules exhibit nanogap-independent conductance in single-molecule junctions",
abstract = "Molecular electronic devices require precise control over the flow of current in single molecules. However, the electron transport properties of single molecules critically depend on dynamic molecular conformations in nanoscale junctions. Here we report a unique strategy for controlling molecular conductance using shape-persistent molecules. Chemically diverse, charged ladder molecules, synthesized via a one-pot multicomponent ladderization strategy, show a molecular conductance (d[log(G/G0)]/dx ≈ −0.1 nm−1) that is nearly independent of junction displacement, in stark contrast to the nanogap-dependent conductance (d[log(G/G0)]/dx ≈ −7 nm−1) observed for non-ladder analogues. Ladder molecules show an unusually narrow distribution of molecular conductance during dynamic junction displacement, which is attributed to the shape-persistent backbone and restricted rotation of terminal anchor groups. These principles are further extended to a butterfly-like molecule, thereby demonstrating the strategy{\textquoteright}s generality for achieving gap-independent conductance. Overall, our work provides important avenues for controlling molecular conductance using shape-persistent molecules. (Figure presented.)",
author = "Xiaolin Liu and Hao Yang and Hassan Harb and Rajarshi Samajdar and Woods, {Toby J.} and Oliver Lin and Qian Chen and Romo, {Adolfo I.B.} and Joaqu{\'i}n Rodr{\'i}guez-L{\'o}pez and Assary, {Rajeev S.} and Moore, {Jeffrey S.} and Schroeder, {Charles M.}",
note = "This research was supported by the US Department of Energy (DE-SC0022035). We express our gratitude to the Mass Spectrometry Laboratory and the 3M Materials Chemistry Laboratory at the University of Illinois for their assistance with mass spectrometry and X-ray experiments, respectively. Major funding for the 500\u2009MHz Bruker CryoProbe was provided by the Roy J. Carver Charitable Trust (Muscatine, Iowa; grant no. 15-4521) to the School of Chemical Sciences NMR Lab. R.S.A. and H.H. acknowledge Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the US Department of Energy under contract no. DE-AC02-06CH11357. H.H. and R.S.A. acknowledge the computing resources provided on \u2018BEBOP\u2019 and \u2018IMPROV\u2019, two computing clusters operated by the Laboratory Computing Resource Center at Argonne National Laboratory. X.L. acknowledges Y. Diao at the University of Illinois Urbana-Champaign for offering the use of the UV\u2013visible spectrophotometer. X.L. acknowledges N. Jackson, B. A. Suslick and R. Zhang at the University of Illinois Urbana-Champaign for constructive suggestions.",
year = "2024",
month = nov,
doi = "10.1038/s41557-024-01619-5",
language = "English (US)",
volume = "16",
pages = "1772--1780",
journal = "Nature Chemistry",
issn = "1755-4330",
publisher = "Nature Publishing Group",
number = "11",
}