Effect of electric field gradient on sub-nanometer spatial resolution of tip-enhanced Raman spectroscopy

Scientific Reports
Lingyan MengMengtao Sun

Abstract

Tip-enhanced Raman spectroscopy (TERS) with sub-nanometer spatial resolution has been recently demonstrated experimentally. However, the physical mechanism underlying is still under discussion. Here we theoretically investigate the electric field gradient of a coupled tip-substrate system. Our calculations suggest that the ultra-high spatial resolution of TERS can be partially attributed to the electric field gradient effect owning to its tighter spatial confinement and sensitivity to the infrared (IR)-active of molecules. Particularly, in the case of TERS of flat-lying H₂TBPP molecules,we find the electric field gradient enhancement is the dominating factor for the high spatial resolution, which qualitatively coincides with previous experimental report. Our theoretical study offers a new paradigm for understanding the mechanisms of the ultra-high spatial resolution demonstrated in tip-enhanced spectroscopy which is of importance but neglected.

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Citations

Apr 3, 2016·The Review of Scientific Instruments·Yurui FangMengtao Sun
Apr 6, 2016·ACS Nano·Alessandro AlabastriPeter Nordlander
Jul 18, 2015·Journal of the American Chemical Society·Sai DuanYi Luo
Aug 30, 2016·Analytical Chemistry·Zhenglong ZhangMengtao Sun
Sep 21, 2016·Journal of Chemical Theory and Computation·Sai DuanYi Luo
Dec 23, 2016·Chemical Reviews·Eric A PozziRichard P Van Duyne
Feb 18, 2017·Chemical Reviews·Xian ShiAchim Hartschuh
May 10, 2017·Chemical Communications : Chem Comm·A Bhattarai, P Z El-Khoury
Nov 12, 2015·Applied Spectroscopy·Lucas LangelüddeckeVolker Deckert
Jun 24, 2017·Chemical Society Reviews·Marie Richard-LacroixVolker Deckert
Jun 24, 2017·Chemical Society Reviews·Tanja Deckert-GaudigVolker Deckert
Jun 28, 2016·Physical Chemistry Chemical Physics : PCCP·Kishore K MadapuSandip Dhara
Mar 1, 2019·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Yong WeiGuangjun Tian
Jan 9, 2018·Nanoscale·Alexander G MilekhinDietrich R T Zahn
May 22, 2017·The Journal of Chemical Physics·Sai DuanYi Luo
Sep 1, 2018·Light, Science & Applications·Song JiangJ G Hou
Jul 1, 2017·Chemical Society Reviews·Song-Yuan DingMartin Moskovits
May 2, 2018·Nature Communications·Chang ChenPol Van Dorpe
Oct 12, 2018·Analytical and Bioanalytical Chemistry·Feng Shao, Renato Zenobi
Nov 11, 2020·The Journal of Chemical Physics·Matthew M SartinBin Ren
Jan 28, 2021·The Journal of Chemical Physics·K FiederlingS Gräfe
Oct 25, 2017·The Journal of Physical Chemistry Letters·Emanuele PolianiJanina Maultzsch
Dec 6, 2017·Nano Letters·Hyun-Hang ShinZee Hwan Kim
Jun 15, 2017·Chemical Reviews·Alyssa B ZrimsekRichard P Van Duyne

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