NC-AFM contrast formation on the calcite ($10\bar {1}4$) surface

Rahe, Philipp; Schütte, Jens; Kühnle, Angelika

doi:10.1088/0953-8984/24/8/084006

Cited by 29 publications

(53 citation statements)

References 50 publications

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“…At various positions in the image, deviations from the periodic lattice of the calcite (10.4) surface can be observed. In previous AFM works, similar atomic-scale inhomogeneities on the calcite surface have been assigned to point defects [7,8,18]. The measurements show that point defects on the surface of calcite (10.4) are present in the sample.…”

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confidence: 57%

Resolving Point Defects in the Hydration Structure of Calcite (10.4) with Three-Dimensional Atomic Force Microscopy

et al. 2018

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It seems natural to assume that defects at mineral surfaces critically influence interfacial processes such as the dissolution and growth of minerals in water. The experimental verification of this claim, however, is challenging and requires real-space methods with utmost spatial resolution, such as atomic force microscopy (AFM). While defects at mineral-water interfaces have been resolved in 2D AFM images before, the perturbation of the surrounding hydration structure has not yet been analyzed experimentally. In this Letter, we demonstrate that point defects on the most stable and naturally abundant calcite (10.4) surface can be resolved using high-resolution 3D AFM-even within the fifth hydration layer. Our analysis of the hydration structure surrounding the point defect shows a perturbation of the hydration with a lateral extent of approximately one unit cell. These experimental results are corroborated by molecular dynamics simulations.

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confidence: 57%

Resolving Point Defects in the Hydration Structure of Calcite (10.4) with Three-Dimensional Atomic Force Microscopy

et al. 2018

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“…For example, even for bare calcite it is known that certain tips image two surface features as a single one (so-called row pairing). 64 Thus, it is possible that we image pairs of molecules aligned sideways. Another option is that the islands were instead formed by flat-laying BPP dimers aligned next to each other.…”

Section: The Journal Of Physical Chemistry C Articlementioning

confidence: 99%

Where Is the Most Hydrophobic Region? Benzopurpurine Self-Assembly at the Calcite–Water Interface

et al. 2017

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Control of molecular self-assembly at solid− liquid interfaces is challenging due to the complex interplay between molecule−molecule, molecule−surface, molecule− solvent, surface−solvent, and solvent−solvent interactions. Here, we use in-situ dynamic atomic force microscopy to study the self-assembly of Benzopurpurine 4B into oblong islands with a highly ordered inner structure yet incommensurate with the underlying calcite (10.4) surface. Molecular dynamics and free energy calculations provide insights by showing that Benzopurpurine 4B molecules do not anchor to the surface directly but instead assemble on top of the second hydration layer. This seemingly peculiar behavior was then rationalized by considering that hydrophobic molecules placed atop the second water layer cause the least distortion to the existing hydration structure. Further experiments for the adsorption of Benzopurpurine 4B on other minerals indicate that the specific interfacial water structure on calcite is decisive for rationalizing the self-assembly of Benzopurpurine 4B in this system.

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“…5 Later, ionic crystal sublattices have been identified on several crystals, including, for example, CaF 2 (111), 6 NiO(001), 7,8 NaCl(001), 9 and calcite (10.4). 10 A particularly challenging system has been studied by Sugimoto et al who have been the first to demonstrate the identification of individual surface atoms in an alloy of Pb, Sn, and Si, even though these atoms occupy identical surface positions and are not oppositely charged. 11 All the above studies have been carried out in UHV.…”

Section: ■ Introductionmentioning

confidence: 99%

Chemical Identification at the Solid–Liquid Interface

et al. 2016

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Solid−liquid interfaces are decisive for a wide range of natural and technological processes, including fields as diverse as geochemistry and environmental science as well as catalysis and corrosion protection. Dynamic atomic force microscopy nowadays provides unparalleled structural insights into solid−liquid interfaces, including the solvation structure above the surface. In contrast, chemical identification of individual interfacial atoms still remains a considerable challenge. So far, an identification of chemically alike atoms in a surface alloy has only been demonstrated under well-controlled ultrahigh vacuum conditions. In liquids, the recent advent of three-dimensional force mapping has opened the potential to discriminate between anionic and cationic surface species. However, a full chemical identification will also include the far more challenging situation of alike interfacial atoms (i.e., with the same net charge). Here we demonstrate the chemical identification capabilities of dynamic atomic force microscopy at solid−liquid interfaces by identifying Ca and Mg cations at the dolomite−water interface. Analyzing site-specific vertical positions of hydration layers and comparing them with molecular dynamics simulations unambiguously unravels the minute but decisive difference in ion hydration and provides a clear means for telling calcium and magnesium ions apart. Our work, thus, demonstrates the chemical identification capabilities of dynamic AFM at the solid−liquid interface.

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NC-AFM contrast formation on the calcite ($10\bar {1}4$) surface

Cited by 29 publications

References 50 publications

Resolving Point Defects in the Hydration Structure of Calcite (10.4) with Three-Dimensional Atomic Force Microscopy

Resolving Point Defects in the Hydration Structure of Calcite (10.4) with Three-Dimensional Atomic Force Microscopy

Where Is the Most Hydrophobic Region? Benzopurpurine Self-Assembly at the Calcite–Water Interface

Chemical Identification at the Solid–Liquid Interface

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