Experimental investigation of the density profile in the liquid-vapor interface of mercury and gallium

Bosio, L.; Cortès, R.; Defrain, A.; Oumezine, Mohamed

doi:10.1016/0022-3093(84)90627-6

Cited by 17 publications

(7 citation statements)

References 10 publications

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“…These measurements confirmed that the liquid/vapor interfacial region is relatively sharp, with no deviations from the average structure extending beyond 10 Å. Although the results of Bosio et al 31 could be modeled with an atomically layered density profile, their coarse resolution allowed an equally good modeling by a monotonic profile, as shown by the authors. For Ga, with an atomic diameter dϳ2.5 Å, the signature of atomic layering is expected to be a peak in the specular reflectivity near q z ϳ2.4 Å Ϫ1 .…”

Section: Introductionsupporting

confidence: 57%

“…For Ga, with an atomic diameter dϳ2.5 Å, the signature of atomic layering is expected to be a peak in the specular reflectivity near q z ϳ2.4 Å Ϫ1 . In addition, Ga readily oxidizes, 32,33 and ultrahigh vacuum ͑UHV͒ and surface cleaning techniques were not employed by Bosio et al 31 but have been utilized by Kawamoto et al 30 and Regan et al 21 The experiments presented here have relied on UHV conditions and measurements that extend out to q z ϳ3 Å Ϫ1 to unambiguously establish surface-induced atomic layering. This approach differs substantially from measurements on Hg, 20 which are simplified by its relatively small reduction potential that consequently allows the surface to be kept oxide free by enclosing it in a reducing atmosphere of H 2 gas.…”

Section: Introductionmentioning

confidence: 99%

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X-ray reflectivity studies of liquid metal and alloy surfaces

et al. 1997

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Surface-induced atomic layering at the liquid/vapor interface in liquid metals has been observed using x-ray reflectivity on sputtered clean surfaces under ultrahigh vacuum conditions. A well-defined quasi-Bragg peak is obtained for surfaces of elemental Ga and a Ga-In alloy at large wave vectors q z ϳ2.3-2.5 Å Ϫ1 . These results are an unambiguous indication of atomic layering with an interlayer spacing dϳ2/q z ϭ2.5-2.7 Å. For liquid Ga, the amplitude of the electron-density oscillations, which is significantly underestimated by existing theory and molecular simulation, decays with a characteristic length of 6 Å, which is twice that of Hg. Results on the alloy show a clear enrichment of indium at the topmost surface layer, consistent with the Gibbs adsorption rule. The enrichment consists of a single monolayer, with subsequent layers at the bulk eutectic composition. In order to suppress mechanically excited surface waves, the measurements were performed on thin liquid metal films (Ͻ0.5 mm deep͒, which leads to a macroscopically curved surface due to the large surface tensions in liquid metals. The experimental challenges posed by measurements on curved surfaces and the techniques that were developed are discussed in detail. ͓S0163-1829͑97͒01324-6͔

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Section: Introductionsupporting

confidence: 57%

Section: Introductionmentioning

confidence: 99%

X-ray reflectivity studies of liquid metal and alloy surfaces

et al. 1997

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“…Though long inaccessible via X-ray probes, recent developments in synchrotron radiation sources delivering intense brilliant X-rays have enabled access to this liquid-liquid interface. X-ray investigations of layering and charge effects provided new insight into the atomic structure specifically (Barton et al, 1986;Bosio et al, 1984;Dimasi et al, 1998;Magnussen et al, 1995;Duval et al, 2012). Studies of interface charge transfer at immiscible liquid-liquid interfaces and nanoparticle growth (Grü nder et al, 2011) are key to understanding these processes and offer interesting applications, for example for the production of nanoparticles by electrodeposition (Carim et al, 2011).…”

Section: Adsorption At the Liquid Mercury-electrolyte Interfacementioning

confidence: 99%

“…Surface X-ray scattering methods belong to the very few experimental approaches that provide such data, even for interfaces between two extended immiscible liquid phases, in situ with atomic scale resolution. For the free surfaces of liquids in contact with a gas phase, extensive studies of the vertical and in-plane structure have been performed by X-ray reflectivity, diffuse X-ray scattering, and grazing-incidence X-ray diffraction, providing a wealth of quantitative results on the surface structure of dielectric (Braslau et al, 1988;Ocko et al, 1994) and metallic liquids (Barton et al, 1986;Bosio et al, 1984;Dimasi et al, 1998;Magnussen et al, 1995), surface segregation (Regan et al, 1997;Shpyrko et al, 2006), surface phase transitions (Deutsch et al, 1995;Wu et al, 1993), and the structure and phase behaviour of organic layers on liquids (Kraack et al, 2002;Magnussen et al, 1996;Weinbach et al, 1994). In contrast, investigations of the deeply buried interfaces between two liquids are scarce and have been performed only for a few selected systems (see, for some examples, Bosio et al, 1984;Duval et al, 2012;Grü nder et al, 2011;Luo et al, 2006;Tamam et al, 2011;Schlossman & Tikhonov, 2008).…”

Section: Introductionmentioning

confidence: 99%

A novel X-ray diffractometer for studies of liquid–liquid interfaces

et al. 2013

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The study of liquid-liquid interfaces with X-ray scattering methods requires special instrumental considerations. A dedicated liquid surface diffractometer employing a tilting double-crystal monochromator in Bragg geometry has been designed. This diffractometer allows reflectivity and grazing-incidence scattering measurements of an immobile mechanically completely decoupled liquid sample, providing high mechanical stability. The available energy range is from 6.4 to 29.4 keV, covering many important absorption edges. The instrument provides access in momentum space out to 2.54 Å(-1) in the surface normal and out to 14.8 Å(-1) in the in-plane direction at 29.4 keV. Owing to its modular design the diffractometer is also suitable for heavy apparatus such as vacuum chambers. The instrument performance is described and examples of X-ray reflectivity studies performed under in situ electrochemical control and on biochemical model systems are given.

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“…Surface X-ray scattering methods can uniquely deliver such dataeven for interfaces between two extended immiscible liquid phasesin situ and operando with an atomic-scale resolution. This was realized as early as in the 1990s; 31 however, X-ray investigations of these deeply buried interfaces were hampered by experimental challenges that make these measurements by far more challenging than X-ray scattering studies of solid-liquid electrodes. These difficulties include mechanical stability, high X-ray absorption and the background and the problem that the sample cannot be tilted, requiring specialized X-ray diffractometers.…”

Section: Introductionmentioning

confidence: 99%

The Atomic scale structure of liquid metal–electrolyte interfaces

2016

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Electrochemical interfaces between immiscible liquids have lately received renewed interest, both for gaining fundamental insight as well as for applications in nanomaterial synthesis. In this feature article we demonstrate that the atomic scale structure of these previously inaccessible interfaces nowadays can be explored by in situ synchrotron based X-ray scattering techniques. Exemplary studies of a prototypical electrochemical system - a liquid mercury electrode in pure NaCl solution - reveal that the liquid metal is terminated by a well-defined atomic layer. This layering decays on length scales of 0.5 nm into the Hg bulk and displays a potential and temperature dependent behaviour that can be explained by electrocapillary effects and contributions of the electronic charge distribution on the electrode. In similar studies of nanomaterial growth, performed for the electrochemical deposition of PbFBr, a complex nucleation and growth behaviour is found, involving a crystalline precursor layer prior to the 3D crystal growth. Operando X-ray scattering measurements provide detailed data on the processes of nanoscale film formation.

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Experimental investigation of the density profile in the liquid-vapor interface of mercury and gallium

Cited by 17 publications

References 10 publications

X-ray reflectivity studies of liquid metal and alloy surfaces

X-ray reflectivity studies of liquid metal and alloy surfaces

A novel X-ray diffractometer for studies of liquid–liquid interfaces

The Atomic scale structure of liquid metal–electrolyte interfaces

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