Intermediate tunnelling-hopping regime in DNA charge transport

Limin Xiang, Julio L. Palma, Christopher Bruot, Vladimiro Mujica, Mark A Ratner, Nongjian Tao

Research output: Contribution to journalArticle

92 Citations (Scopus)

Abstract

Charge transport in molecular systems, including DNA, is involved in many basic chemical and biological processes, and its understanding is critical if they are to be used in electronic devices. This important phenomenon is often described as either coherent tunnelling over a short distance or incoherent hopping over a long distance. Here, we show evidence of an intermediate regime where coherent and incoherent processes coexist in double-stranded DNA. We measure charge transport in single DNA molecules bridged to two electrodes as a function of DNA sequence and length. In general, the resistance of DNA increases linearly with length, as expected for incoherent hopping. However, for DNA sequences with stacked guanine-cytosine (GC) base pairs, a periodic oscillation is superimposed on the linear length dependence, indicating partial coherent transport. This result is supported by the finding of strong delocalization of the highest occupied molecular orbitals of GC by theoretical simulation and by modelling based on the Büttiker theory of partial coherent charge transport.

Original languageEnglish
Pages (from-to)221-226
Number of pages6
JournalNature Chemistry
Volume7
Issue number3
DOIs
Publication statusPublished - 2015

Fingerprint

Charge transfer
DNA
DNA sequences
Cytosine
Guanine
Chemical Phenomena
Biological Phenomena
Molecular orbitals
Base Pairing
Electrodes
Equipment and Supplies
Molecules

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)
  • Medicine(all)

Cite this

Intermediate tunnelling-hopping regime in DNA charge transport. / Xiang, Limin; Palma, Julio L.; Bruot, Christopher; Mujica, Vladimiro; Ratner, Mark A; Tao, Nongjian.

In: Nature Chemistry, Vol. 7, No. 3, 2015, p. 221-226.

Research output: Contribution to journalArticle

Xiang, Limin ; Palma, Julio L. ; Bruot, Christopher ; Mujica, Vladimiro ; Ratner, Mark A ; Tao, Nongjian. / Intermediate tunnelling-hopping regime in DNA charge transport. In: Nature Chemistry. 2015 ; Vol. 7, No. 3. pp. 221-226.
@article{1cc1dc56412548a68bd380150242b256,
title = "Intermediate tunnelling-hopping regime in DNA charge transport",
abstract = "Charge transport in molecular systems, including DNA, is involved in many basic chemical and biological processes, and its understanding is critical if they are to be used in electronic devices. This important phenomenon is often described as either coherent tunnelling over a short distance or incoherent hopping over a long distance. Here, we show evidence of an intermediate regime where coherent and incoherent processes coexist in double-stranded DNA. We measure charge transport in single DNA molecules bridged to two electrodes as a function of DNA sequence and length. In general, the resistance of DNA increases linearly with length, as expected for incoherent hopping. However, for DNA sequences with stacked guanine-cytosine (GC) base pairs, a periodic oscillation is superimposed on the linear length dependence, indicating partial coherent transport. This result is supported by the finding of strong delocalization of the highest occupied molecular orbitals of GC by theoretical simulation and by modelling based on the B{\"u}ttiker theory of partial coherent charge transport.",
author = "Limin Xiang and Palma, {Julio L.} and Christopher Bruot and Vladimiro Mujica and Ratner, {Mark A} and Nongjian Tao",
year = "2015",
doi = "10.1038/nchem.2183",
language = "English",
volume = "7",
pages = "221--226",
journal = "Nature Chemistry",
issn = "1755-4330",
publisher = "Nature Publishing Group",
number = "3",

}

TY - JOUR

T1 - Intermediate tunnelling-hopping regime in DNA charge transport

AU - Xiang, Limin

AU - Palma, Julio L.

AU - Bruot, Christopher

AU - Mujica, Vladimiro

AU - Ratner, Mark A

AU - Tao, Nongjian

PY - 2015

Y1 - 2015

N2 - Charge transport in molecular systems, including DNA, is involved in many basic chemical and biological processes, and its understanding is critical if they are to be used in electronic devices. This important phenomenon is often described as either coherent tunnelling over a short distance or incoherent hopping over a long distance. Here, we show evidence of an intermediate regime where coherent and incoherent processes coexist in double-stranded DNA. We measure charge transport in single DNA molecules bridged to two electrodes as a function of DNA sequence and length. In general, the resistance of DNA increases linearly with length, as expected for incoherent hopping. However, for DNA sequences with stacked guanine-cytosine (GC) base pairs, a periodic oscillation is superimposed on the linear length dependence, indicating partial coherent transport. This result is supported by the finding of strong delocalization of the highest occupied molecular orbitals of GC by theoretical simulation and by modelling based on the Büttiker theory of partial coherent charge transport.

AB - Charge transport in molecular systems, including DNA, is involved in many basic chemical and biological processes, and its understanding is critical if they are to be used in electronic devices. This important phenomenon is often described as either coherent tunnelling over a short distance or incoherent hopping over a long distance. Here, we show evidence of an intermediate regime where coherent and incoherent processes coexist in double-stranded DNA. We measure charge transport in single DNA molecules bridged to two electrodes as a function of DNA sequence and length. In general, the resistance of DNA increases linearly with length, as expected for incoherent hopping. However, for DNA sequences with stacked guanine-cytosine (GC) base pairs, a periodic oscillation is superimposed on the linear length dependence, indicating partial coherent transport. This result is supported by the finding of strong delocalization of the highest occupied molecular orbitals of GC by theoretical simulation and by modelling based on the Büttiker theory of partial coherent charge transport.

UR - http://www.scopus.com/inward/record.url?scp=84923370994&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84923370994&partnerID=8YFLogxK

U2 - 10.1038/nchem.2183

DO - 10.1038/nchem.2183

M3 - Article

C2 - 25698331

AN - SCOPUS:84923370994

VL - 7

SP - 221

EP - 226

JO - Nature Chemistry

JF - Nature Chemistry

SN - 1755-4330

IS - 3

ER -