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Nature Nanotechnology 13, 371–375 (2018)

Quantitative assessment of intermolecular interactions by atomic force microscopy imaging using copper oxide tips

Harry Mönig1,2,*, Saeed Amirjalayer1,2, Alexander Timmer1,2, Zhixin Hu3, Lacheng Liu1,2, Oscar Díaz Arado1,2, Marvin Cnudde1,2, Cristian Alejandro Strassert1,2, Wei Ji4, Michael Rohlfing5 and Harald Fuchs1,2

1 Physikalisches Institut, Westfälische Wilhelms-Universität Münster, Münster, Germany.

2 Center for Nanotechnology, Münster, Germany.

3 Center for Joint Quantum Studies and Department of Physics, Tianjin University, Tianjin, China.

4 Department of Physics and Beijing Key Laboratory of Optoelectronic Functional Materials & Micro-Nano Devices, Renmin University of China, Beijing, China.

5 Institut für Festkörpertheorie, Westfälische Wilhelms-Universität Münster, Münster, Germany.

* Corresponding Authors:  Mönig, Harry(harry.moenig@uni-muenster.de)

Abstract

Atomic force microscopy is an impressive tool with which to directly resolve the bonding structure of organic compounds1–5 . The methodology usually involves chemical passivation of the probe-tip termination by attaching single molecules or atoms such as CO or Xe (refs 1,6–9). However, these probe particles are only weakly connected to the metallic apex, which results in considerable dynamic deflection. This probe particle deflection leads to pronounced image distortions, systematic overestimation of bond lengths, and in some cases even spurious bond-like contrast features, thus inhibiting reliable data interpretation8–12. Recently, an alternative approach to tip passivation has been used in which slightly indenting a tip into oxidized copper substrates and subsequent contrast analysis allows for the verification of an oxygen-terminated Cu tip13–15. Here we show that, due to the covalently bound configuration of the terminal oxygen atom, this copper oxide tip (CuOx tip) has a high structural stability, allowing not only a quantitative determination of individual bond lengths and access to bond order effects, but also reliable intermolecular bond characterization. In particular, by removing the previous limitations of flexible probe particles, we are able to provide conclusive experimental evidence for an unusual intermolecular N–Au–N three-centre bond. Furthermore, we demonstrate that CuOx tips allow the characterization of the strength and configuration of individual hydrogen bonds within a molecular assembly.

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Center for Joint Quantum Studies, School of Science, Tianjin University     Address : Yaguan Road 135, Jinnan District, 300350 Tianjin, P. R. China