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This thesis focuses on the synthesis of novel functional materials based on plasmonic nanoparticles. Three systems with targeted surface modification and functionalization have been designed and synthesized, involving modified perylenediimide doped silica-coated silver nanowires, polydopamine or TiO2 coated gold-palladium nanorods and thiolated poly(ethylene glycol) (PEG-SH)/dodecanethiol (DDT) modified silver nanospheres. Their possible applications as plasmonic resonators, chiral sensors as well as photo-catalysts have been studied. In addition, the interaction between silver nanospheres and 2,3,5,6-Tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ) molecules has also been investigated in detail.
In the first part of the thesis, surface modification on Ag nanowires (NWs) with optimized silica coating through a modified Stöber method has been firstly conducted, employing sodium hydroxide (NaOH) to replace ammonia solution (NH4OH). The coated silver nanowires with a smooth silica shell have been investigated by single-particle dark-field scattering spectroscopy, transmission electron microscopy and electron-energy loss spectroscopy to characterize the morphologies and structural components. The silica-coated silver nanowires can be further functionalized with fluorescent molecules in the silica shell via a facile one-step coating method. The as-synthesized nanowire is further coupled with a gold nanosphere by spin-coating for the application of the sub-diffractional chiral sensor for the first time. The exciton-plasmon-photon interconversion in the system eases the signal detection in the perfectly matched 1D nanostructure and contributes to the high contrast of the subwavelength chiral sensing for the polarized light.
In the second part of the thesis, dumbbell-shaped Au-Pd nanorods coated with a layer of polydopamine (PDA) or titanium dioxide (TiO2) have been constructed. The PDA- and TiO2- coated Au-Pd nanorods show a strong photothermal conversion performance under NIR illumination. Moreover, the catalytic performance of the particles has been investigated using the reduction of 4-nitrophenol (4-NP) as the model reaction. Under light irradiation, the PDA-coated Au-Pd nanorods exhibit a superior catalytic activity by increasing the reaction rate constant of 3 times. The Arrhenius-like behavior of the reaction with similar activation energies in the presence and absence of light irradiation indicates the photoheating effect to be the dominant mechanism of the reaction acceleration. Thus, we attribute the enhanced performance of the catalysis to the strong photothermal effect that is driven by the optical excitation of the gold surface plasmon as well as the synergy with the PDA layer.
In the third part, the kinetic study on the adsorption of 2,3,5,6-Tetrafluoro-7,7,8,8-tetracyanoquino-dimethane (F4TCNQ) on the surface of Ag nanoparticles (Ag NPs) in chloroform has been reported in detail. Based on the results obtained from the UV-vis-NIR absorption spectroscopy, cryogenic transmission electron microscopy (cryo-TEM), scanning nano-beam electron diffraction (NBED) and electron energy loss spectroscopy (EELS), a two-step interaction kinetics has been proposed for the Ag NPs and F4TCNQ molecules. It includes the first step of electron transfer from Ag NPs to F4TCNQ indicated by the ionization of F4TCNQ, and the second step of the formation of Ag-F4TCNQ complex. The whole process has been followed via UV-vis-NIR absorption spectroscopy, which reveals distinct kinetics at two stages: the instantaneous ionization and the long-term complex formation. The kinetics and the influence of the molar ratio of Ag NPs/F4TCNQ molecules on the interaction between Ag NPs and F4TCNQ molecules in the organic solution are reported herein for the first time. Furthermore, the control experiment with silica-coated Ag NPs indicates that the charge transfer at the surface between Ag NPs and F4TCNQ molecules has been prohibited by a silica layer of 18 nm.
In this study, the kinetics of the adsorption of 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F(4)TCNQ) on the surface of Ag nanoparticles (Ag NPs) in chloroform has been intensively investigated, as molecular doping is known to play a crucial role in organic electronic devices. Based on the results obtained from UV-visible (vis)-near-infrared (NIR) absorption spectroscopy, cryogenic transmission electron microscopy, scanning nanobeam electron diffraction, and electron energy loss spectroscopy, a two-step interaction kinetics has been proposed for the Ag NPs and F(4)TCNQ molecules, which includes the first step of electron transfer from Ag NPs to F(4)TCNQ indicated by the ionization of F(4)TCNQ and the second step of the formation of a Ag-F(4)TCNQ complex. The whole process has been followed via UV-vis-NIR absorption spectroscopy, which reveals distinct kinetics at two stages: the instantaneous ionization and the long-term complex formation. The kinetics and the influence of the molar ratio of Ag NPs/F(4)TCNQ molecules on the interaction between Ag NPs and F(4)TCNQ molecules in an organic solution are reported herein for the first time. Furthermore, the control experiment with silica-coated Ag NPs manifests that the charge transfer at the surface between Ag NPs and F(4)TCNQ molecules is prohibited by a silica layer of 18 nm.
Abstract
In recent years, feedforward neural networks (NNs) have been successfully applied to reconstruct global plasmasphere dynamics in the equatorial plane. These neural network‐based models capture the large‐scale dynamics of the plasmasphere, such as plume formation and erosion of the plasmasphere on the nightside. However, their performance depends strongly on the availability of training data. When the data coverage is limited or non‐existent, as occurs during geomagnetic storms, the performance of NNs significantly decreases, as networks inherently cannot learn from the limited number of examples. This limitation can be overcome by employing physics‐based modeling during strong geomagnetic storms. Physics‐based models show a stable performance during periods of disturbed geomagnetic activity if they are correctly initialized and configured. In this study, we illustrate how to combine the neural network‐ and physics‐based models of the plasmasphere in an optimal way by using data assimilation. The proposed approach utilizes advantages of both neural network‐ and physics‐based modeling and produces global plasma density reconstructions for both quiet and disturbed geomagnetic activity, including extreme geomagnetic storms. We validate the models quantitatively by comparing their output to the in‐situ density measurements from RBSP‐A for an 18‐month out‐of‐sample period from June 30, 2016 to January 01, 2018 and computing performance metrics. To validate the global density reconstructions qualitatively, we compare them to the IMAGE EUV images of the He+ particle distribution in the Earth's plasmasphere for a number of events in the past, including the Halloween storm in 2003.
We investigate the transition from incoherence to global collective motion in a three-dimensional swarming model of agents with helical trajectories, subject to noise and global coupling. Without noise this model was recently proposed as a generalization of the Kuramoto model and it was found that alignment of the velocities occurs discontinuously for arbitrarily small attractive coupling. Adding noise to the system resolves this singular limit and leads to a continuous transition, either to a directed collective motion or to center-of-mass rotations.
Sulfated biomolecules are known to influence numerous biological processes in all living organisms. Particularly, they contribute to prevent and inhibit the hypercoagulation condition. The failure of polymeric implants and blood contacting devices is often related to hypercoagulation and microbial contamination. Here, bioactive sulfated biomacromolecules are mimicked by sulfation of poly(glycerol glycidyl ether) (polyGGE) films. Autoclaving, gamma-ray irradiation and ethylene oxide (EtO) gas sterilization techniques were applied to functionalized materials. The sulfate group density and hydrophilicity of sulfated polymers were decreased while chain mobility and thermal degradation were enhanced post autoclaving when compared to those after EtO sterilization. These results suggest that a quality control after sterilization is mandatory to ensure the amount and functionality of functionalized groups are retained.
This study investigated how touching and being touched by a humanoid robot affects human physiology, impressions of the interaction, and attitudes towards humanoid robots. 21 healthy adult participants completed a 3 (touch style: touching, being touched, pointing) x 2 (body part: hand vs buttock) within-subject design using a Pepper robot. Skin conductance response (SCR) was measured during each interaction. Perceived impressions of the interaction (i.e., friendliness, comfort, arousal) were measured per questionnaire after each interaction. Participants' demographics and their attitude towards robots were also considered. We found shorter SCR rise times in the being touched compared to the touching condition, possibly reflecting psychological alertness to the unpredictability of robot-initiated contacts. The hand condition had shorter rise times than the buttock condition. Most participants evaluated the hand condition as most friendly and comfortable and the robot-initiated interactions as most arousing. Interacting with Pepper improved attitudes towards robots. Our findings require future studies with larger samples and improved procedures. They have implications for robot design in all domains involving tactile interactions, such as caring and intimacy.
The within-site variability in site response is the randomness in site response at a given site from different earthquakes and is treated as aleatory variability in current seismic hazard/risk analyses.
In this study, we investigate the single-station variability in linear site response at K-NET and KiK-net stations in Japan using a large number of earthquake recordings.
We found that the standard deviation of the horizontal-to-vertical Fourier spectral ratio at individual sites, that is single-station horizontal-to-vertical spectral ratio (HVSR) sigma sigma(HV,s), approximates the within-site variability in site response quantified using surface-to-borehole spectral ratios (for oscillator frequencies higher than the site fundamental frequency) or empirical ground-motion models.
Based on this finding, we then utilize the single-station HVSR sigma as a convenient tool to study the site-response variability at 697 KiK-net and 1169 K-NET sites.
Our results show that at certain frequencies, stiff, rough and shallow sites, as well as small and local events tend to have a higher sigma(HV,s).
However, when being averaged over different sites, the single-station HVSR sigma, that is sigma(HV), increases gradually with decreasing frequency. In the frequency range of 0.25-25 Hz, sigma(HV) is centred at 0.23-0.43 in ln scales (a linear scale factor of 1.26-1.54) with one standard deviation of less than 0.1. sigma(HV) is quite stable across different tectonic regions, and we present a constant, as well as earthquake magnitude- and distance-dependent sigma(HV) models.
Mechanical behaviors of granite after thermal treatment under loading and unloading conditions
(2021)
Understanding the mechanical behaviors of granite after thermal treatment under loading and unloading conditions is of utmost relevance to deep geothermal energy recovery. In the present study, a series of loading and unloading triaxial compression tests (20, 40 and 60 MPa) on granite specimens after exposure to different temperatures (20, 200, 300, 400, 500 and 600 degrees C) was carried out to quantify the combined effects of thermal treatment and loading/unloading stress conditions on granite strength and deformation. Changes in the microstructure of granite exposed to high temperatures were revealed by optical microscopy. The experimental results indicate that both, thermal treatment and loading/unloading stress conditions, degrade the mechanical behaviors and further decrease the carrying capacity of granite. The gradual degradation of the mechanical characteristics of granite after thermal treatment is mainly associated with the evolution of thermal micro-cracks based on optical microscopy observations. The unloading stress state induces the extension of tension cracks parallel to the axial direction, and thus, the mechanical properties are degraded. Temperatures above 400 degrees C have a more significant influence on the mechanical characteristics of granite than the unloading treatment, whereby 400 degrees C can be treated as a threshold temperature for the delineation of significant deterioration. This study is expected to support feasibility and risk assessments by means of providing data for analytical calculations and numerical simulations on granite exposed to high temperatures during geothermal energy extraction.
As overconsumption has negative effects on ecological balance, social equality, and individual well-being, reducing consumption levels among the materially affluent is an emerging strategy for sustainable development. Today's youth form a crucial target group for intervening in unsustainable overconsumption habits and for setting the path and ideas on responsible living. This article explores young people's motivations for engaging in three behavioural patterns linked to anti-consumption (voluntary simplicity, collaborative consumption, and living within one's means) in relation to sustainability. Applying a qualitative approach, laddering interviews reveal the consequences and values behind the anti-consumption behaviours of young people of ages 14 to 24 according to a means-end chains analysis. The findings highlight potential for and the challenges involved in motivating young people to reduce material levels of consumption for the sake of sustainability. Related consumer policy tools from the fields of education and communication are identified. This article provides practical implications for policy makers, activists, and educators. Consumer policies may strengthen anti-consumption among young people by addressing individual benefits, enabling reflection on personal values, and referencing credible narratives. The presented insights can help give a voice to young consumers, who struggle to establish themselves as key players in shaping the future consumption regime.
Would the world be a better place if one were to adopt a European approach to state immunity?
(2021)
This chapter argues not only that there is no European Sonderweg (or ‘special way’) when it comes to the law of state immunity but that there ought not to be one. Debates within The Hague Conference on Private International Law in the late 1990s and those leading to the adoption of the 2002 UN Convention on Jurisdictional Immunities of States, as well as the development of the EU Brussels Regulation on Jurisdiction and Enforcement, as amended in 2015, all demonstrate that state immunity was not meant to be limited by such treaties but ‘safeguarded’. Likewise, there is no proof that regional European customary law limits state immunity when it comes to ius cogens violations, as Italy and (partly) Greece are the only European states denying state immunity in such cases while the European Court of Human Rights has, time and again, upheld a broad concept of state immunity. It therefore seems unlikely that in the foreseeable future a specific European customary law norm on state immunity will develop, especially given the lack of participation in such practice by those states most concerned by the matter, including Germany. This chapter considers the possible legal implications of the jurisprudence of the Italian Constitutional Court for European military operations (if such operations went beyond peacekeeping). These implications would mainly depend on the question of attribution: if one where to assume that acts undertaken within the framework of military operations led by the EU were to be, at least also, attributable to the troop-contributing member states, the respective troop-contributing state would be entitled to enjoy state immunity exactly to the same degree as in any kind of unilateral military operations. Additionally, some possible perspectives beyond Sentenza 238/2014 are examined, in particular concerning the redress awarded by domestic courts ‘as long as’ neither the German nor the international system grant equivalent protection to the victims of serious violations of international humanitarian law committed during World War II. In the author’s opinion, strengthening the jurisdiction of international courts and tribunals, bringing interstate cases for damages before the International Court of Justice, as well as providing for claims commissions where individual compensation might be sought for violations of international humanitarian law would be more useful and appropriate mechanisms than denying state immunity.