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Register a new userMonitoring morphological and chemical properties during silver solid-state dewetting
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Solid-state dewetting phenomenon in silver thin films offers a straightforward method to obtain structures having controlled shape or size -this latter in principle spanning several orders of magnitudes -- with potentially strong interest in many applications involving high-tech industry and biomedicine. In this work nanostructured silver is deposited by pulsed electron ablation technique and its surface modified upon thermal treatments in air at increasing temperatures. Surface chemistry and morphology are then monitored simultaneously by X-ray photoemission spectroscopy and atomic force microscopy; in particular, the power spectral density of surface heights is used to analyze the alteration of morphology induced by annealing. It is shown that this approach adds a level of information about the dewetting process since it allows to separate between long- and short-range surface behavior and to retrieve statistical quantities relevant to a description of the features in view of applications. Our results are presented in the framework of a multidisciplinary approach, advantages and limits of which are deepened and discussed.
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Materials featuring anomalous suppression of density fluctuations over large length scales are emerging systems known as disordered hyperuniform. The underlying hidden order renders them appealing for several applications, such as light management and topologically protected electronic states. These applications require scalable fabrication, which is hard to achieve with available top-down approaches. Theoretically, it is known that spinodal decomposition can lead to disordered hyperuniform architectures. Spontaneous formation of stable patterns could thus be a viable path for the bottom-up fabrication of these materials. Here we show that mono-crystalline semiconductor-based structures, in particular Si$_{1-x}$Ge$_{x}$ layers deposited on silicon-on-insulator substrates, can undergo spinodal solid-state dewetting featuring correlated disorder with an effective hyperuniform character. Nano- to micro-metric sized structures targeting specific morphologies and hyperuniform character can be obtained, proving the generality of the approach and paving the way for technological applications of disordered hyperuniform metamaterials. Phase-field simulations explain the underlying non-linear dynamics and the physical origin of the emerging patterns.
Galvanic replacement reactions on metal nanoparticles are often used for the preparation of hollow nanostructures with tunable porosity and chemical composition, leading to tailored optical and catalytic properties. However, the precise interplay between the three-dimensional (3D) morphology and chemical composition of nanostructures during Galvanic replacement is not always well understood as the 3D chemical imaging of nanoscale materials is still challenging. It is especially far from straightforward to obtain detailed information from the inside of hollow nanostructures using electron microscopy techniques such as SEM or TEM. We demonstrate here that a combination of state-of-the-art EDX mapping with electron tomography results in the unambiguous determination of both morphology transformation and elemental composition of nanostructures in 3D, during Galvanic replacement of Ag nanocubes. This work provides direct and unambiguous experimental evidence leading to new insights in the understanding of the galvanic replacement reaction. In addition, the powerful approach presented here can be applied to a wide range of nanoscale transformation processes, which will undoubtedly guide the development of novel nanostructures.
One of the main challenges of the sintering of sterling silver is the phenomenon of swelling causing de-densification and a considerable reduction of the sintering kinetics. This swelling phenomenon opposes sintering and it needs to be addressed by a well-controlled processing atmosphere. In the present study, the pressure-less sintering behavior of sterling silver is investigated in air, argon, and vacuum. A specially modified spark plasma sintering mold is designed to study the pressure-less sintering of sterling silver in a high vacuum environment. The conducted analysis is extended to the new constitutive equations of sintering enabling the prediction of the swelling phenomena and the identification of the internal equivalent pressure that opposes the sintering.
Plasmonics offers an enticing platform to manipulate light at the subwavelength scale. Currently, loss represents the most serious challenge impeding its progress and broad impact towards practical technology. In this regard, silver (Ag) is by far the preferred plasmonic material at optical frequencies, having the lowest loss among all metals in this frequency range. However, large discrepancies exist among widely quoted values of optical loss in Ag due to variations in sample preparation procedures that produce uncontrollable grain boundaries and defects associated with additional loss. A natural question arises: what are the intrinsic fundamental optical properties of Ag and its ultimate possibilities in the field of plasmonics? Using atomically-smooth epitaxial Ag films, we extracted new optical constants that reflect significantly reduced loss and measured greatly enhanced propagation distance of surface plasmon polaritons (SPPs) beyond what was previously considered possible. By establishing a new benchmark in the ultimate optical properties of Ag, these results will have a broad impact for metamaterials and plasmonic applications.
Based on the work of Gritsenko et al. (GLLB) [Phys. Rev. A 51, 1944 (1995)], the method of Kuisma et al. [Phys. Rev. B 82, 115106 (2010)] to calculate the band gap in solids was shown to be much more accurate than the common local density approximation (LDA) and generalized gradient approximation (GGA). The main feature of the GLLB-SC potential (SC stands for solid and correlation) is to lead to a nonzero derivative discontinuity that can be conveniently calculated and then added to the Kohn-Sham band gap for a comparison with the experimental band gap. In this work, a thorough comparison of GLLB-SC with other methods, e.g., the modified Becke-Johnson (mBJ) potential [F. Tran and P. Blaha, Phys. Rev. Lett. 102, 226401 (2009)], for electronic, magnetic, and density-related properties is presented. It is shown that for the band gap, GLLB-SC does not perform as well as mBJ for systems with a small band gap and strongly correlated systems, but is on average of similar accuracy as hybrid functionals. The results on itinerant metals indicate that GLLB-SC overestimates significantly the magnetic moment (much more than mBJ does), but leads to excellent results for the electric field gradient, for which mBJ is in general not recommended. In the aim of improving the results, variants of the GLLB-SC potential are also tested.
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