A universal signature in the melting of metallic nanoparticles

Delgado-Callico, Laia; Rossi, Kevin; Pinto-Miles, Raphael; Salzbrenner, Pascal T.; Baletto, Francesca

doi:10.1039/d0nr06850k

Cited by 25 publications

(26 citation statements)

References 76 publications

(97 reference statements)

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“…This observation holds regardless of whether they lie in the inner part or at the surface of the NP, and their coordination. Furthermore, this result confirms and rationalizes the universal signature of melting for the whole NP we recently proposed 13 .…”

Section: Resultssupporting

confidence: 90%

“…The first concerns the difficulty of defining an unbiased characterization of the phase change mechanism. Indeed, the identification of order parameters to characterize solid–liquid phase changes at the nanoscale is an active topic of debate with a long tradition 10 – 13 . Widely used methods often rely on chemical-intuition and heuristic approaches, and can therefore lead to descriptive order parameters, which are neither fully general nor robust to parameter tuning.…”

Section: Introductionmentioning

confidence: 99%

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Data-driven simulation and characterisation of gold nanoparticle melting

et al. 2021

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The simulation and analysis of the thermal stability of nanoparticles, a stepping stone towards their application in technological devices, require fast and accurate force fields, in conjunction with effective characterisation methods. In this work, we develop efficient, transferable, and interpretable machine learning force fields for gold nanoparticles based on data gathered from Density Functional Theory calculations. We use them to investigate the thermodynamic stability of gold nanoparticles of different sizes (1 to 6 nm), containing up to 6266 atoms, concerning a solid-liquid phase change through molecular dynamics simulations. We predict nanoparticle melting temperatures in good agreement with available experimental data. Furthermore, we characterize the solid-liquid phase change mechanism employing an unsupervised learning scheme to categorize local atomic environments. We thus provide a data-driven definition of liquid atomic arrangements in the inner and surface regions of a nanoparticle and employ it to show that melting initiates at the outer layers.

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Section: Resultssupporting

confidence: 90%

Section: Introductionmentioning

confidence: 99%

Data-driven simulation and characterisation of gold nanoparticle melting

et al. 2021

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“…For this reason, we directly contrast the simulated spectra with the experimental curve, using the Kullback-Leibler (D KL ) divergence, which quantifies how much two curves differ from each other. D KL is zero for identical curves, and increases the more they diverge [48]. Therefore, we can assign geometries by comparing D KL -1 values; a better agreement between experiment and calculation is reflected in a larger D KL -1 value.…”

Section: Resultsmentioning

confidence: 98%

“…D KL is zero for identical curves, and increases the more they diverge. 48 Therefore, we can assign geometries by comparing D KL −1 values; a better agreement between experiment and calculation is reflected in a larger D KL −1 value. For this procedure, the computed vibrational modes of a specific isomer were used to construct a simulated IR spectrum, in which Gaussian functions were assumed centered at each vibrational frequency.…”

Section: Resultsmentioning

confidence: 99%

The size-dependent influence of palladium doping on the structures of cationic gold clusters

et al. 2021

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“…The Kullback–Leibler divergence is zero when both distributions are identical, and increases the more they diverge from each other [ 39 ]. Using this analysis to quantify the hybridization between Au and Ar gives the values 3.18, 3.40 and 3.51, for Au 3 Ar + , Au 15 Ar + and Au 16 Ar + , respectively.…”

Section: Discussionmentioning

confidence: 99%

Argon Adsorption on Cationic Gold Clusters Aun+ (n ≤ 20)

Ferrari¹,

Janssens²

2021

Molecules

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The interaction of Aun+ (n ≤ 20) clusters with Ar is investigated by combining mass spectrometric experiments and density functional theory calculations. We show that the inert Ar atom forms relatively strong bonds with Aun+. The strength of the bond strongly varies with the cluster size and is governed by a fine interplay between geometry and electronic structure. The chemical bond between Aun+ and Ar involves electron transfer from Ar to Au, and a stronger interaction is found when the Au adsorption site has a higher positive partial charge, which depends on the cluster geometry. Au15+ is a peculiar cluster size, which stands out for its much stronger interaction with Ar than its neighbors, signaled by a higher abundance in mass spectra and a larger Ar adsorption energy. This is shown to be a consequence of a low-coordinated Au adsorption site in Au15+, which possesses a large positive partial charge.

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A universal signature in the melting of metallic nanoparticles

Abstract: We unveil a universal feature in the distribution of the atomic-pair distances that characterizes the melting of monometallic nanoparticles, in vacuum or in a strongly interacting environment, regardless of their size, shape, and composition.

Cited by 25 publications

References 76 publications

Data-driven simulation and characterisation of gold nanoparticle melting

Data-driven simulation and characterisation of gold nanoparticle melting

The size-dependent influence of palladium doping on the structures of cationic gold clusters

Argon Adsorption on Cationic Gold Clusters Aun+ (n ≤ 20)

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