Benchmarking atomically defined AFM tips for chemical-selective imaging

Lammers, Bertram Schulze; Yesilpinar, Damla; Timmer, Alexander; Hu, Zhixin; Ji, Wei; Amirjalayer, Saeed; Fuchs, Harald; Mönig, Harry

doi:10.1039/d1nr04080d

Cited by 6 publications

(15 citation statements)

References 46 publications

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“…A related high chemical reactivity of these N-Cu-N sites, specifically toward oxygen, is furthermore supported by their observed strong interaction with the O-terminated copper tip used in the nc-AFM measurements. 42 In many single atom catalysis approaches, metal atoms are stabilized on top of carbon-based materials through nitrogen atoms. 43,44 Therefore, we investigated potential electrocatalytic activity of the N-Cu-N sites of the copper nitride structures toward the oxygen reduction reaction (ORR).…”

Section: Resultsmentioning

confidence: 99%

“…All AFM images are recorded with an atomically defined Oterminated copper tip, which was functionalized on a (2×1)Oreconstructed Cu(110) surface by indentation of 1−8 Å. 29,30,42 The intactness of the functionalized tip after measuring the prepared sample is controlled by subsequent unambiguous contrast analysis on the (2×1)O-reconstructed Cu(110) surface. 35,42 The shown SPM data is processed and filtered by the Scanning Probe Image Processor, SPIP5.1.…”

Section: Associated Contentmentioning

confidence: 99%

“…29,30,42 The intactness of the functionalized tip after measuring the prepared sample is controlled by subsequent unambiguous contrast analysis on the (2×1)O-reconstructed Cu(110) surface. 35,42 The shown SPM data is processed and filtered by the Scanning Probe Image Processor, SPIP5.1. Slightly Gaussian-filtered images are shown with absolute Δf values in the color bar, whereas for Laplace of Gaussian-filtered images no quantitative values are given.…”

Section: Associated Contentmentioning

confidence: 99%

“…For nc-AFM images, an atomically defined Oterminated copper tip was used, which is formed by controlled indentation of 1−8 Å into an (2×1)O-reconstructed Cu(110) surface. 29,30,42 Computation Details. Electronic structure calculations were performed in the framework of density functional theory (DFT) using the projector augmented wave method (PAW) 80 as implemented in the Vienna Ab Initio Simulation Package (VASP).…”

Section: Associated Contentmentioning

confidence: 99%

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Real-Space Identification of Non-Noble Single Atomic Catalytic Sites within Metal-Coordinated Supramolecular Networks

et al. 2022

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With regard to the development of single atom catalysts (SACs), non-noble metal–organic layers combine a large functional variability with cost efficiency. Here, we characterize reacted layers of melamine and melem molecules on a Cu(111) surface by noncontact atomic force microscopy (nc-AFM), X-ray photoelectron spectroscopy (XPS) and ab initio simulations. Upon deposition on the substrate and subsequent heat treatments in ultrahigh vacuum (UHV), these precursors undergo a stepwise dehydrogenation. After full dehydrogenation of the amino groups, the molecular units lie flat and are strongly chemisorbed on the copper substrate. We observe a particularly extreme interaction of the dehydrogenated nitrogen atoms with single copper atoms located at intermolecular sites. In agreement with the nc-AFM measurements performed with an O-terminated copper tip on these triazine- and heptazine-based copper nitride structures, our ab initio simulations confirm a pronounced interaction of oxygen species at these N–Cu–N sites. To investigate the related functional properties of our samples regarding the oxygen reduction reaction (ORR), we developed an electrochemical setup for cyclic voltammetry experiments performed at ambient pressure within a drop of electrolyte in a controlled O2 or N2 environment. Both copper nitride structures show a robust activity in irreversibly catalyzing the reduction of oxygen. The activity is assigned to the intermolecular N–Cu–N sites of the triazine- and heptazine-based copper nitrides or corresponding oxygenated versions (N–CuO–N, N–CuO2–N). By combining nc-AFM characterization on the atomic scale with a direct electrochemical proof of performance, our work provides fundamental insights about active sites in a technologically highly relevant reaction.

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Section: Resultsmentioning

confidence: 99%

Section: Associated Contentmentioning

confidence: 99%

Section: Associated Contentmentioning

confidence: 99%

Section: Associated Contentmentioning

confidence: 99%

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Real-Space Identification of Non-Noble Single Atomic Catalytic Sites within Metal-Coordinated Supramolecular Networks

et al. 2022

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“…[8][9][10][11][12][13][14][15][16][17][18][19] Therefore, the bond imaging technique became an inevitable tool for deciphering the mechanisms of on-surface synthesis. 20,21 Experimentally, submolecular resolution is commonly achieved by utilizing qPlus sensors 22 with CO-functionalized tips 23,24 that are mechanically actuated close to their fundamental resonance ( f 1 ) in ultra-high vacuum conditions at low temperature ( p < 10 −10 mbar, T ≈ 5.2 K). The images are usually obtained in constant-height or constant-current mode 25 by tracking changes in the fundamental frequency of the sensor 26 that are caused by short range interactions between the CO tip and the atoms of the imaged molecule.…”

Section: Introductionmentioning

confidence: 99%

Chemical bond imaging using torsional and flexural higher eigenmodes of qPlus sensors

et al. 2022

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How Water Binds to Microcline Feldspar (001)

Franceschi,

Conti,

Lezuo

et al. 2023

J. Phys. Chem. Lett.

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Microcline feldspar (KAlSi 3 O 8 ) is a common mineral with important roles in Earth's ecological balance. It participates in carbon, potassium, and water cycles, contributing to CO 2 sequestration, soil formation, and atmospheric ice nucleation. To understand the fundamentals of these processes, it is essential to establish microcline's surface atomic structure and its interaction with the omnipresent water molecules. This work presents atomic-scale results on microcline's lowest-energy surface and its interaction with water, combining ultrahigh vacuum investigations by noncontact atomic force microscopy and X-ray photoelectron spectroscopy with density functional theory calculations. An ordered array of hydroxyls bonded to silicon or aluminum readily forms on the cleaved surface at room temperature. The distinct proton affinities of these hydroxyls influence the arrangement and orientation of the first water molecules binding to the surface, holding potential implications for the subsequent condensation of water.

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Benchmarking atomically defined AFM tips for chemical-selective imaging

Abstract: Controlling the identity of the tip-terminating atom or molecule in low-temperature atomic force microscopy has led to ground breaking progress in surface chemistry and nanotechnology. Lacking a comparative tip-performance assessment,...

Cited by 6 publications

References 46 publications

Real-Space Identification of Non-Noble Single Atomic Catalytic Sites within Metal-Coordinated Supramolecular Networks

Real-Space Identification of Non-Noble Single Atomic Catalytic Sites within Metal-Coordinated Supramolecular Networks

Chemical bond imaging using torsional and flexural higher eigenmodes of qPlus sensors

How Water Binds to Microcline Feldspar (001)

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