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Chin. Phys. B, 2020, Vol. 29(11): 116803    DOI: 10.1088/1674-1056/aba9d0
Special Issue: SPECIAL TOPIC — Water at molecular level
TOPICAL REVIEW—Water at molecular level Prev   Next  

Atomic-level characterization of liquid/solid interface

Jiani Hong(洪嘉妮)1 and Ying Jiang(江颖)1,2,3, †
1 International Center for Quantum Materials, School of Physics, Peking University, Beijing 100871, China
2 Collaborative Innovation Center of Quantum Matter, Beijing 100871, China
3 CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing 100190, China

The detailed understanding of various underlying processes at liquid/solid interfaces requires the development of interface-sensitive and high-resolution experimental techniques with atomic precision. In this perspective, we review the recent advances in studying the liquid/solid interfaces at atomic level by electrochemical scanning tunneling microscope (EC-STM), non-contact atomic force microscopy (NC-AFM), and surface-sensitive vibrational spectroscopies. Different from the ultrahigh vacuum and cryogenic experiments, these techniques are all operated in situ under ambient condition, making the measurements close to the native state of the liquid/solid interface. In the end, we present some perspectives on emerging techniques, which can defeat the limitation of existing imaging and spectroscopic methods in the characterization of liquid/solid interfaces.

Keywords:  liquid/solid interface      atomic scale      scanning tunneling microscope (STM)      atomic force microscopy (AFM)  
Received:  08 May 2020      Revised:  06 July 2020      Accepted manuscript online:  28 July 2020
Corresponding Authors:  Corresponding author. E-mail:   

Cite this article: 

Jiani Hong(洪嘉妮) and Ying Jiang(江颖) Atomic-level characterization of liquid/solid interface 2020 Chin. Phys. B 29 116803

Fig. 1.  

(a) The configuration of EC-STM, where the bipotentiostat controls the potential of the substrate (WE1), STM tip (WE2), and counter electrode (CE) with respect to the reference electrode (RE). The majority of STM tip is coated with insulation. (b)–(c) Schematic diagram of the concept of detecting catalytic sites. The tunnelling barrier varies with the change of local environment between the STM tip and sample, arising from the attachment and detachment of reactants and products. Tunnelling-current noise is larger in the case of scanning over a step shown in (c) than that over a terrace in (b), suggesting that step sites are more active than terrace steps, and the noise is reflected on the z-position when STM is operated in constant-current mode. (d) Constant-height STM image of the boundary between a Pd island and Au (111) substrate under hydrogen evolution reaction (HER) conditions in 0.1 M sulfuric acid. (e) Detailed tunnelling-current line scans for the boundary shown in (d). Panels (b)–(e) reproduced with permission from Ref. [92]

Fig. 2.  

(a) 3D AFM image of aqueous KCl/mica interface in the case of low molarity (0.2 M KCl). A monolayer of K+ (red color) is absorbed on mica topped by two hydration layers (0.3 nm thick), which follow the corrugation of substrate (lighter stripes). (b) XZ frame of (a) (raw data). The ordered layer at interface is very thin (below 1.0 nm). (c) XY frame taken at z = 0.34 nm. The structure of the water molecules in the 2nd hydration layer is revealed. The origin of z is chosen at the mica surface (minima in (b)). (d) 3D AFM image of aqueous KCl/mica interface for high molarity (4 M KCl). Interfacial layers can be divided into two regions, ordered liquid layers (2 nm thick) and bulk liquid above it. (e) XZ frame of (d) (low pass filtered image). An ordered liquid layer extending up to 2–3 nm from the mica at high molarities is characterized at the interface. The inset shows a filtered image (FFT) of the bottom right corner of the XZ frame. (f) XZ frame extending 5 nm above the mica surface. Reproduced with permission from Ref. [143].

Fig. 3.  

(a)–(b) 3D FM-AFM image and MD simulation on the water/clinochlore (001) interface across an area including the T, BII, and BI regions shown in (k), respectively. (c)–(f) Experimental lateral 2D force maps and theoretical lateral 2D-normalized water (oxygen) density maps of 1st and 2nd layers on T region, respectively. Honeycomb-like pattern of the first hydration layer and a dot-like pattern of the second hydration layer were observed both in AFM experiments and simulations. (g)–(l) Lateral 2D force maps and theoretical lateral 2D-normalized water (oxygen) density maps of 1st and 2nd layer on BI region, respectively. Atomic-scale patterns of both layers observed in experiments and simulations show the same lattice constant. (k)–(l) Topographic image and structural model around the step edge, respectively. Adsorbed water molecules are represented as red dots in (l). (m) XZ force maps along the broken lines P–Q and R–S in (l). Reproduced with permission from Ref. [158].

Fig. 4.  

(a) Illustration of two regions at the charged water interface. (b) OH stretching spectra of the BIL of the lignoceric acid monolayer-water interface at three different pH values. At pH = 2.5 (the neutral interface), a negative OH stretching band below 3350 cm−1 extending beyond 3000 cm−1 dominates, arising from down-pointing OH of water and COOH in the fatty acid headgroups. At pH = 12 (nearly fully deprotonated interface), a broad positive band from 3000 cm−1 to 3450 cm−1 dominates, resulting from up-pointing OH of water molecules donor bonded to O of COO. (c)–(d) Side-view snapshots of the MD trajectories for the neutral and fully deprotonated fatty acid–water interfaces, respectively. (e) Schematic illustration of in situ electrochemical shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS). (f) Potential-dependent evolution of the hydrogen-bond network of interfacial water. (g) Schematic of the EC-TERS operando measurement. Oxidation OFF state: left, 1.1 V vs. Pd-H. Oxidation ON state: right, 1.45 V vs. Pd-H. (h) Two kinds of EC-TER spectra recorded at different AuOx defect locations and fitted by Gaussian peaks. (i) EC-TERS map in the region of catalytic defects. (j) Schematic illustration of the difference in AuOx peak position. Panels (a)–(d) reproduced with permission from Ref. [179], (e)–(f) reproduced with permission from Ref. [187], and (g)–(j) reproduced with permission from Ref. [195].

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