Engineering nanometre-scale coherence in soft matter

Chaoren Liu, Limin Xiang, Yuqi Zhang, Peng Zhang, David N. Beratan, Yueqi Li, Nongjian Tao

Research output: Contribution to journalArticlepeer-review

49 Scopus citations

Abstract

Electronic delocalization in redox-active polymers may be disrupted by the heterogeneity of the environment that surrounds each monomer. When the differences in monomer redox-potential induced by the environment are small (as compared with the monomer-monomer electronic interactions), delocalization persists. Here we show that guanine (G) runs in double-stranded DNA support delocalization over 4-5 guanine bases. The weak interaction between delocalized G blocks on opposite DNA strands is known to support partially coherent long-range charge transport. The molecular-resolution model developed here finds that the coherence among these G blocks follows an even-odd orbital-symmetry rule and predicts that weakening the interaction between G blocks exaggerates the resistance oscillations. These findings indicate how sequence can be exploited to change the balance between coherent and incoherent transport. The predictions are tested and confirmed using break-junction experiments. Thus, tailored orbital symmetry and structural fluctuations may be used to produce coherent transport with a length scale of multiple nanometres in soft-matter assemblies, a length scale comparable to that of small proteins.

Original languageEnglish (US)
Pages (from-to)941-945
Number of pages5
JournalNature Chemistry
Volume8
Issue number10
DOIs
StatePublished - Oct 1 2016

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

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