Transport processes in directional solidification and their effects on microstructure development

The processing of materials with unique electronic, mechanical, optical and thermal properties plays a crucial role in modern technology. The quality of these materials depend strongly on the microstructures and the solute/dopant fields in the solid product, that are strongly influenced by the intricate coupling of heat and mass transfer and melt flow in the growth systems. An integrated research program is developed that include precisely characterized experiments and detailed physical and numerical modeling of the complex transport and dynamical processes. Direct numerical simulation of the solidification process is carried out that takes into account the unsteady thermo-solutal convection in the vertical Bridgman crystal growth system, and accurately models the thermal interaction between the furnace and the ampoule by appropriately using experimentally measured thermal profiles. The flow instabilities and transitions and the nonlinear evolution following the transitions are investigated by time series and flow pattern analysis. A range of complex dynamical behavior is predicted with increasing thermal Rayleigh number. The route to chaos appears as: steady convection → transient mono-periodic → transient bi-periodic → transient quasiperiodic → transient intermittent oscillation-relaxation → stable intermittent oscillation-relaxation attractor;The spatio-temporal dynamics of the melt flow is found to be directly related to the spatial patterns observed experimentally in the solidified crystals. The application of the model to two phase Sn-Cd peritectic alloys showed that a new class of tree-like oscillating microstructure develops in the solid phase due to unsteady thermo-solutal convection in the liquid melt. These oscillating layered structures can give the illusion of band structures on a plane of polish. The model is applied to single phase solidification in the Al-Cu and Pb-Sn systems to characterize the effect of convection on the macroscopic shape and disorder in the primary arm spacing of the cellular/dendritic freezing front. The apparently puzzling experimental observation of higher disorder in the weakly convective Al-Cu system than that in the highly convective Pb-Sn system is explained by the numerical calculations

Direct growth of 2D and 3D graphene nano-structures over large glass substrates by tuning a sacrificial Cu-template layer

We demonstrate direct growth of two-dimensional (2D) and three-dimensional (3D) graphene structures on glass substrates. By starting from catalytic copper nanoparticles of different densities and using chemical vapour deposition (CVD) techniques, different 2D and 3D morphologies can be obtained, including graphene sponge-like, nano-ball and conformal graphene structures. More important, we show that the initial copper template can be completely removed via sublimation during CVD and, if need be, subsequent metal etching. This allows optical transmissions close to the bare substrate, which, combined with electrical conductivity make the proposed technique very attractive for creating graphene with high surface to volume ratio for a wide variety of applications, including antiglare display screens, solar cells, light-emitting diodes, gas and biological plasmonic sensors.Peer ReviewedPostprint (author's final draft

Functionalized surfaces with tailored wettability determine Influenza A infectivity

Surfaces contaminated with pathogenic microorganisms contribute to their transmission and spreading. The development of 'active surfaces' that can reduce or eliminate this contamination necessitates a detailed understanding of the molecular mechanisms of interactions between the surfaces and the microorganisms. Few studies have shown that, among the different surface characteristics, the wetting properties play an important role in reducing virus infectivity. Here, we systematically tailored the wetting characteristics of flat and nanostructured glass surfaces by functionalizing them with alkyl- and fluoro-silanes. We studied the effects of these functionalized surfaces on the infectivity of Influenza A viruses using a number of experimental and computational methods including real-time fluorescence microscopy and molecular dynamics simulations. Overall, we show that surfaces that are simultaneously hydrophobic and oleophilic are more efficient in deactivating enveloped viruses. Our results suggest that the deactivation mechanism likely involves disruption of the viral membrane upon its contact with the alkyl chains. Moreover, enhancing these specific wetting characteristics by surface nanostructuring led to an increased deactivation of viruses. These combined features make these substrates highly promising for applications in hospitals and similar infrastructures where antiviral surfaces can be crucial

Dry transfer of graphene to dielectrics and flexible substrates using polyimide as a transparent and stable intermediate layer

We demonstrate the direct transfer of graphene from Cu foil to glass and flexible substrates such as PET, using polyimide (PI) mixed with an aminosilane (3-aminopropyltrimethoxysilane) or only PI, respectively, as intermediate layer. We probe the scalability and roll-to-roll processing of this technique by using two different equipment: hot press and a laminator. High quality, clean and continuous areas of graphene monolayer can be transferred with the advantage of Cu recycling for future growth catalyst as it is peeled-off mechanically from the substrate/PI/graphene structure. More important are the high transparency of the samples together with the electron doping achieved (n<sub>S</sub>= 0.21 to 4 x 10<sup>13</sup> cm<sup>-2</sup>), as the performing graphene face is not in direct contact with PMMA, PI or other materials, and the high mobility (µ<sub>H</sub> up to 1250 cm<sup>2</sup>/Vcenterdots). Stability of the structure in terms of sheet resistance (R<sub>S</sub>) at high temperatures, bending cycles and water immersion make this technique promising for future applications and implementation at the large scale.Postprint (author's final draft

Transport processes in directional solidification and their effects on microstructure development

The processing of materials with unique electronic, mechanical, optical and thermal properties plays a crucial role in modern technology. The quality of these materials depend strongly on the microstructure and the solute/dopant fields in the solid product, that are strongly influenced by the intricate coupling of heat and mass transfer and melt flow in the growth systems. An integrated research program is developed that include precisely characterized experiments and detailed physical and numerical modeling of the complex transport and dynamical processes. Direct numerical simulation of the solidification process is carried out that takes into account the unsteady thermo-solutal convection in the vertical Bridgman crystal growth system, and accurately models the thermal interaction between the furnace and the ampoule by appropriately using experimentally measured thermal profiles. The flow instabilities and transitions and the nonlinear evolution following the transitions are investigated by time series and flow pattern analysis. A range of complex dynamical behavior is predicted with increasing thermal Rayleigh number. The route to chaos appears as: steady convection {r_arrow} transient mono-periodic {r_arrow} transient bi-periodic {r_arrow} transient quasi-periodic {r_arrow} transient intermittent oscillation-relaxation {r_arrow} stable intermittent oscillation-relaxation attractor. The spatio-temporal dynamics of the melt flow is found to be directly related to the spatial patterns observed experimentally in the solidified crystals. The application of the model to two phase Sn-Cd peritectic alloys showed that a new class of tree-like oscillating microstructure develops in the solid phase due to unsteady thermo-solutal convection in the liquid melt. These oscillating layered structures can give the illusion of band structures on a plane of polish. The model is applied to single phase solidification in the Al-Cu and Pb-Sn systems to characterize the effect of convection on the macroscopic shape and disorder in the primary arm spacing of the cellular/dendritic freezing front. The apparently puzzling experimental observation of higher disorder in the weakly convective Al-Cu system than that in the highly convective Pb-Sn system is explained by the numerical calculations

Dynamics of pulsed laminar jets

Bibliography: p. 150-155

Transport processes in directional solidification and their effects on microstructure development

The processing of materials with unique electronic, mechanical, optical and thermal properties plays a crucial role in modern technology. The quality of these materials depend strongly on the microstructures and the solute/dopant fields in the solid product, that are strongly influenced by the intricate coupling of heat and mass transfer and melt flow in the growth systems. An integrated research program is developed that include precisely characterized experiments and detailed physical and numerical modeling of the complex transport and dynamical processes. Direct numerical simulation of the solidification process is carried out that takes into account the unsteady thermo-solutal convection in the vertical Bridgman crystal growth system, and accurately models the thermal interaction between the furnace and the ampoule by appropriately using experimentally measured thermal profiles. The flow instabilities and transitions and the nonlinear evolution following the transitions are investigated by time series and flow pattern analysis. A range of complex dynamical behavior is predicted with increasing thermal Rayleigh number. The route to chaos appears as: steady convection → transient mono-periodic → transient bi-periodic → transient quasiperiodic → transient intermittent oscillation-relaxation → stable intermittent oscillation-relaxation attractor;The spatio-temporal dynamics of the melt flow is found to be directly related to the spatial patterns observed experimentally in the solidified crystals. The application of the model to two phase Sn-Cd peritectic alloys showed that a new class of tree-like oscillating microstructure develops in the solid phase due to unsteady thermo-solutal convection in the liquid melt. These oscillating layered structures can give the illusion of band structures on a plane of polish. The model is applied to single phase solidification in the Al-Cu and Pb-Sn systems to characterize the effect of convection on the macroscopic shape and disorder in the primary arm spacing of the cellular/dendritic freezing front. The apparently puzzling experimental observation of higher disorder in the weakly convective Al-Cu system than that in the highly convective Pb-Sn system is explained by the numerical calculations.</p

Transparent Glass Surfaces with Silica Nanopillars for Radiative Cooling

The increasing global use of cooling systems and the need of reducing greenhouse effect are pushing the emergence of more efficient cooling methods. In particular, passive radiative cooling technology extracts heat from objects by tailoring their optical emissivity using surface micro- and nanostructuring. Being capable of increasing thermal emissivity is especially relevant for widespread glass structures and devices, e.g., displays, car and building windows, and solar cells. In this paper, we propose a scalable lithography-free nanostructuring method to increase the infrared (IR) emissivity of glass by reducing the high reflection associated with the SiO2 Reststrahlen band around 9 μm wavelength. Furthermore, we show that with an additional thin polymer coating the scattering (haze) in the visible due to the deep nanostructures can be dramatically reduced while maintaining the large IR emissivity. We experimentally prove that our nanostructured surface can extract more heat via radiation emission than the bare glass substrate, while keeping full transparency

Tuning of Ultra-Thin Gold Films by Photoreduction

Ultrathin metal films (UTMFs) are used in a wide range of applications, from transparent electrodes to infrared mirrors and metasurfaces. Due to their small thickness (<5 nm), the electrical and optical properties of UTMFs can be changed by external stimuli, for example, by applying an electric field through an ion gel. It is also known that oxidized thin films and nanostructures of Au can be reduced by irradiating with short-wavelength light. Here we show that the resistance, reflectance, and resonant optical response of Au UTMFs is changed significantly by ultraviolet light. More specifically, photoreduction and oxidation processes can be sequentially applied for continuous tuning, with observed modulation ranges for sheet resistance (Rs) and reflectance of more than 40% and 30%, respectively. The proposed method has the potential for achieving reconfigurable UTMF structures and trimming their response to specific working points, e.g., a predetermined resonance wavelength and amplitude. This is also important for large scale deployment of such surfaces as one can compensate material nonuniformity, morphological, and structural dimension errors occurring during fabrication.This work was partially funded by CEX2019-000910-S [MCIN/AEI/10.13039/501100011033], and the project TUNA-SURF (PID2019-106892RB-I00) from Fundació Cellex, Fundació Mir-Puig, and Generalitat de Catalunya through CERCA and Agència de Gestió d’Ajuts Universitaris i de Recerca (2021 SGR 01458). This project received funding from the European Unio’s Horizon 2020 Research and Innovation Programme under Marie Skłodowska-Curie grant agreement No. 754510, and from Ayuda (PRE2017-082781) funded by MCIN/AEI/10.13039/501100011033 y FSE “El FSE invierte en tu futuro”. This project received funding from the Spanish Ministerio de Ciencia e Innovación through grant PID2019-106860GB-I00/AEI/10.13039/501100011033 and FUNFUTURE (CEX2019-000917-S, Spanish Severo Ochoa Centre of Excellence program). J.M.C. acknowledges FPI fellowships (PRE2020-09411) from MICINN cofinanced by the European Social Fund and the Ph.D. program in Materials Science from Universitat Autònoma de Barcelona.With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).Peer reviewe