Real-space imaging of interfacial water with submolecular resolution

Guo, Jing; Meng, Xiangzhi; Chen, Ji; Peng, Jinbo; Sheng, Jiming; Li, Xinzheng; Xu, Limei; Shi, Junren; Wang, Enge; Jiang, Ying

doi:10.1038/nmat3848

Cited by 183 publications

(149 citation statements)

References 39 publications

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“…The tetramers observed in this work have exactly the same structure as the ones built by tip manipulation at 5 K. Our previous STM and DFT studies reveal that each water molecule donates and accepts just one H bond resulting in a cyclic tetramer, whereas the other four free OH bonds point obliquely upward away from the surface (Fig. 2b,c) 30 . Such a tetramer structure is similar to the one proposed in ref.…”

Section: Resultssupporting

confidence: 74%

“…The deposition of NaCl on a Au(111) surface at room temperature leads to the formation of bilayer (001)-terminated islands with perfect non-polar step edges via a carpet-like growth mode ( Fig. 1a; for experimental details see Methods section) 30,31 . The bilayer NaCl island has a thickness of B5.5 Å such that the electrons from STM tip are still able to tunnel through the insulating films and drain into the Au substrate.…”

Section: Resultsmentioning

confidence: 99%

“…24. It is worthy to note that the tetramer actually contains two degenerate chiral H-bonded loops, which can be distinguished through orbital imaging 30 .…”

Section: Resultsmentioning

confidence: 99%

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An unconventional bilayer ice structure on a NaCl(001) film

et al. 2014

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Water-solid interactions are of broad importance both in nature and technology. The hexagonal bilayer model based on the Bernal-Fowler-Pauling ice rules has been widely adopted to describe water structuring at interfaces. Using a cryogenic scanning tunnelling microscope, here we report a new type of two-dimensional ice-like bilayer structure built from cyclic water tetramers on an insulating NaCl(001) film, which is completely beyond this conventional bilayer picture. A novel bridging mechanism allows the interconnection of water tetramers to form chains, flakes and eventually a two-dimensional extended ice bilayer containing a regular array of Bjerrum D-type defects. Ab initio density functional theory calculations substantiate this bridging growth mode and reveal a striking proton-disordered ice structure. The formation of the periodic Bjerrum defects with unusually high density may have a crucial role as H donor sites in directing multilayer ice growth and in catalysing heterogeneous chemical reactions on water-coated salt surfaces.

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Section: Resultssupporting

confidence: 74%

Section: Resultsmentioning

confidence: 99%

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An unconventional bilayer ice structure on a NaCl(001) film

et al. 2014

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“…A recent article has revealed the HOMO and LUMO of water molecules on Au(111) at 5 K [114]. Similar method could also be applied to detect proton tunneling through the H-bonds.…”

Section: Electronic Delocalization In H-bond Systemsmentioning

confidence: 98%

The electron density delocalization of hydrogen bond systems

Zhang

Jiang

et al. 2018

Advances in Physics: X

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Recent experimental and theoretical researches have gradually proved that hydrogen bond (H-bond) interactions are not simple traditionally considered electrostatic interaction. Instead, they involve electron density delocalization. In this work, we outline the studies of electronic structures of the H-bond systems in water systems and biological organic molecules systems. Theoretical researches based on the first-principles method have found important evidences for electron density delocalization in H-bond region. Topological analysis based on natural bond orbital (NBO) analysis proves that during the formation of the H-bonds, electrons transfer from B orbitals to A-H antibond orbitals. Energy decomposition analyses revealed that the delocalized electronic structures show strong relations with orbital interactions. Moreover, penetrating molecular orbitals (MOs) are proved to contribute to the electron density delocalization of the H-bonds, and the quantitative contributions for such MOs could be obtained with the electronic density projected integral (EDPI) method. The electronic delocalization and the corresponding penetrating MOs could be visualized in water clusters, based on the firstprinciples method. These researches open a new sight for understanding the electronic structures of H-bonds from atomic level, and even contribute to further controlling proton tunneling as well as charge and energy transfer processes.

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“…(2) Coordination recovers as water molecules tend to recover their unoccupied neighbors, reserving energetically favorable sp 3 bonding configurations of oxygen [68,69]. (3) O:H phonon resonant coupling occurs when two pieces of ice are brought contact, as noted by Krim [6].…”

Section: High Friction Coefficient Of Ice On Icementioning

confidence: 99%

From ice superlubricity to quantum friction: Electronic repulsivity and phononic elasticity

Zhang

Huang

et al. 2015

Friction

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Superlubricity means non-sticky and frictionless when two bodies are set contacting motion. Although this occurrence has been extensively investigated since 1859 when Faraday firstly proposed a quasiliquid skin on ice, the mechanism behind the superlubricity remains uncertain. This report features a consistent understanding of the superlubricity pertaining to the slipperiness of ice, self-lubrication of dry solids, and aqueous lubricancy from the perspective of skin bond-electron-phonon adaptive relaxation. The presence of nonbonding electron polarization, atomic or molecular undercoordination, and solute ionic electrification of the hydrogen bond as an addition, ensures the superlubricity. Nonbond vibration creates soft phonons of high magnitude and low frequency with extraordinary adaptivity and recoverability of deformation. Molecular undercoordination shortens the covalent bond with local charge densification, which in turn polarizes the nonbonding electrons making them localized dipoles. The locally pinned dipoles provide force opposing contact, mimicking magnetic levitation and hovercraft. O:H−O bond electrification by aqueous ions has the same effect of molecular undercoordination but it is throughout the entire body of the lubricant. Such a Coulomb repulsivity due to the negatively charged skins and elastic adaptivity due to soft nonbonding phonons of one of the contacting objects not only lowers the effective contacting force but also prevents charge from being transited between the counterparts of the contact. Consistency between theory predictions and observations evidences the validity of the proposal of interface elastic Coulomb repulsion that serves as the rule for the superlubricity of ice, wet and dry frictions, which also reconciles the superhydrophobicity, superlubricity, and supersolidity at contacts.

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Real-space imaging of interfacial water with submolecular resolution

Cited by 183 publications

References 39 publications

An unconventional bilayer ice structure on a NaCl(001) film

An unconventional bilayer ice structure on a NaCl(001) film

The electron density delocalization of hydrogen bond systems

From ice superlubricity to quantum friction: Electronic repulsivity and phononic elasticity

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