Single-molecule sensing of environmental pH--an STM break junction and NEGF-DFT approach

Angewandte Chemie
Zhihai LiEric Borguet

Abstract

Sensors play a significant role in the detection of toxic species and explosives, and in the remote control of chemical processes. In this work, we report a single-molecule-based pH switch/sensor that exploits the sensitivity of dye molecules to environmental pH to build metal-molecule-metal (m-M-m) devices using the scanning tunneling microscopy (STM) break junction technique. Dyes undergo pH-induced electronic modulation due to reversible structural transformation between a conjugated and a nonconjugated form, resulting in a change in the HOMO-LUMO gap. The dye-mediated m-M-m devices react to environmental pH with a high on/off ratio (≈100:1) of device conductivity. Density functional theory (DFT) calculations, carried out under the non-equilibrium Green's function (NEGF) framework, model charge transport through these molecules in the two possible forms and confirm that the HOMO-LUMO gap of dyes is nearly twice as large in the nonconjugated form as in the conjugated form.

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Citations

Jun 7, 2015·Annual Review of Analytical Chemistry·Richard J Nichols, Simon J Higgins
Nov 22, 2016·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Sepideh AfsariEric Borguet
Oct 4, 2014·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Hendrik Schlicke, Carmen Herrmann
Sep 27, 2018·Nanoscale·Xunshan LiuShi-Xia Liu
Jan 29, 2019·Angewandte Chemie·Shuning CaiWenjing Hong
Feb 24, 2015·Nature Communications·Zhihai LiEric Borguet
Jun 10, 2014·Chemistry, an Asian Journal·Lin WangLi-Jun Wan
May 9, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Yousuke OyamaMunetaka Akita
Sep 7, 2017·Topics in Current Chemistry·Takashi Tamaki, Takuji Ogawa
May 12, 2017·Topics in Current Chemistry·Zihao LiuXuefeng Guo
Jun 27, 2019·Angewandte Chemie·Sepideh AfsariEric Borguet
Feb 4, 2021·Physical Chemistry Chemical Physics : PCCP·Manuel Smeu, Kevin Leung
Jul 14, 2021·Angewandte Chemie·Yong HuWenjing Hong
Jan 23, 2018·Nano Letters·Richard J BrookeWalther Schwarzacher
Apr 24, 2020·Journal of the American Chemical Society·Zhi-Hao ZhaoLi-Jun Wan
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