DOI: 10.1126/science.1083825. A Bond-Fluctuation Mechanism for Stochastic Switching in Wired Molecules

A Bond-Fluctuation Mechanism for Stochastic Switching in Wired Molecules

10.1126/science.1083825

Crossref journal-article

American Association for the Advancement of Science (AAAS)

Science (221)

Abstract

Stochastic on-off conductivity switching observed in phenylene-ethynylene oligomers has been explained in terms of changes in ring conformations, or electron localization, or both. We report the observation of stochastic on-off switching in the simplest of wired molecules: octanedithiol, decanedithiol, and dodecanedithiol bonded on an Au(111) surface. Stochastic switching was observed even when a top gold contact was pressed on by a conducting atomic force microscope tip at constant force. The rate of switching increased substantially at 60°C, a temperature at which these films are commonly annealed. Because such switching in alkanethiols is unlikely to be caused by internal molecular electronic changes and cannot be fully accounted for by breaking of the top contact, we argue that the cause is the well-known mobility of molecules tethered to gold via a thiol linkage.

Bibliography

Ramachandran, G. K., Hopson, T. J., Rawlett, A. M., Nagahara, L. A., Primak, A., & Lindsay, S. M. (2003). A Bond-Fluctuation Mechanism for Stochastic Switching in Wired Molecules. Science, 300(5624), 1413â1416.

Authors 6

Ganesh K. Ramachandran (first)
Theresa J. Hopson (additional)
Adam M. Rawlett (additional)
Larry A. Nagahara (additional)
Alex Primak (additional)
Stuart M. Lindsay (additional)

References 28 Referenced 387

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A. O. Solak, S. Ranganathan, T. Itoh, R. L. McCreery, Electr. Solid State Lett.5, E43 (2002). (10.1149/1.1490716) / Electr. Solid State Lett. (2002)
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Alkanemonothiol CH 3 (CH 2 ) n -SH self-assembling monolayers were prepared by incubating freshly annealed epitaxial Au(111) surfaces (Molecular Imaging Phoenix AZ) in 1-mM solutions of toluene or ethanol for 12 to 14 hours. C12d was synthesized as described elsewhere ( 23 ). For insertion of the alkane dithiols the films were rinsed and then incubated in 1-mM dithiol solutions for 8 hours. PETB was prepared as described elsewhere ( 10 ). The insertion of PETB was achieved by placing the rinsed Au(111) film in a 0.5-mM solution of the molecule in distilled tetrahydrofuran and ammonium hydroxide (10 μl) for 30 min in an inert particulate-free glove box. Gold NPs (1.5 nm in diameter) were prepared as described in ( 21 ). Molecules studied with the gold NPs attachment were prepared by rinsing of the dithiol-inserted film followed by incubation in a solution of methylene chloride or tetrahydrofuran (THF) (1 mg of NPs per 30 ml). All films were thoroughly rinsed in toluene (and in methylene chloride if necessary) before measurement. Conducting AFM and STM experiments were performed in liquid cells under toluene in a controlled Ar atmosphere using a PicoSPM microscope (Molecular Imaging). The set point bias and tunnel currents were –1.00 V and 12 pA –0.75 V and 18 pA 0.75 V and 6.5 pA –1.0 V and 15.0 pA –1.0 V and 7.5 pA and –1.0 V and 15.0 pA for C8d C10d C12d C12d-Au PETB and PETB-Au respectively.
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The height of the gold NPs was smaller than might be expected if the conductivity of the PETB molecular wire were much larger on a per-carbon basis than that of the surrounding alkanethiols. However experiments ( 10 ) on single molecules with attached NPs show that this is not the case.
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See the supporting information on Science Online.
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10.1021/cr9502357
Supported by a Nanoscale Interdisciplinary Research Teams award of NSF. We thank D. Gust A. Moore T. Moore O. F. Sankey J. Tomfohr X. Zarate G. Kada R. Tsui and H. Goronkin for helpful discussions and J. Robinson for assistance with data analysis.

Dates

Type	When
Created	22 years, 2 months ago (May 29, 2003, 4:06 p.m.)
Deposited	1 year, 7 months ago (Jan. 9, 2024, 11:21 p.m.)
Indexed	1 month ago (July 20, 2025, 6:43 p.m.)
Issued	22 years, 2 months ago (May 30, 2003)
Published	22 years, 2 months ago (May 30, 2003)
Published Print	22 years, 2 months ago (May 30, 2003)

Funders 0

None

BibTeX

@article{Ramachandran_2003, title={A Bond-Fluctuation Mechanism for Stochastic Switching in Wired Molecules}, volume={300}, ISSN={1095-9203}, url={http://dx.doi.org/10.1126/science.1083825}, DOI={10.1126/science.1083825}, number={5624}, journal={Science}, publisher={American Association for the Advancement of Science (AAAS)}, author={Ramachandran, Ganesh K. and Hopson, Theresa J. and Rawlett, Adam M. and Nagahara, Larry A. and Primak, Alex and Lindsay, Stuart M.}, year={2003}, month=may, pages={1413–1416} }

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