Browsing by Author "Schmidt, Matthias"

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    Sedimentation of binary mixtures: Phase stacking and Nonequilibrium dynamics
    (Hannover : Technische Informationsbibliothek, 2024-12-30) Schmidt, Matthias; de las Heras, Daniel
    Based on equilibrium sedimentation path theory and the local density functional approximation, we investigated the effects of gravity on several relevant types of binary colloidal mixtures. Settled systems are represented by so-called sedimentation paths, which determine the variation of the species-resolved chemical potentials with altitude. Analysing the resulting line segments in the plane of chemical potentials of the bulk phase diagram allows one to rationalize the full equilibrium stacking phenomenology for a given system under gravity. The approach predicts theoretically the stacking sequences of colloidal rod-plate mixtures that were observed in iconic experiments by van der Kooij and Lekkerkerker. Thereby the occurrence of up to five simultaneous phase layers emerges naturally from the mere interplay of gravity and two-phase bulk coexistence, without invoking particle polydispersity. We studied the effects on equilibrium phase stacking upon varying the buoyant mass ratio of both components and our predictions are testable in experiments by systematic variation of the height of sedimentation columns. We have carried out similar sedimentation studies for: plate-spheres mixtures, mass-polydisperse systems, and hard spherocylinders. We suggest that microscopic particle properties, such as the buoyant mass, can be inferred from macroscopic measurements of layer thicknesses in phase stacking sequences. We addressed gravity-induced nonequilibrium flow and structure formation on the basis of power functional theory, adaptive Brownian dynamics computer simulations, and functional machine learning. Power functional theory allows one to rationalize and to model the nonequilibrium behaviour of many-body systems based on the one-body density and velocity field. We have used the approach to categorize systematically the different types of relevant nonequilibrium force contributions and have developed corresponding analytical gradient approximations. Neural functionals, as trained on the basis of both equilibrium and nonequilibrium computer simulation data, were shown to yield accurate predictions for structure formation and design of nonequilibrium flow. We have formulated force-based density functional theory and have demonstrated that neural density functionals outperform the best available hard sphere fundamental measure functionals. We have developed adaptive Brownian dynamics as a performant and highly stable numerical integration scheme for the temporal integration of overdamped many-body Langevin equations of motion, as demonstrated for a particle gel subject to convective sedimentation flow. We have put forward general frameworks for fluctuations of general hyperobservables, for their associated hyperforce correlation functions, and for the gauge invariance of statistical mechanics, where Noether's theorem yields exact sum rules that constrain correlations, as exemplified for ideal and for active sedimentation.
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    Surface cleaning and sample carrier for complementary high-resolution imaging techniques
    (Melville, NY : AIP, 2020) Benettoni, Pietro; Ye, Jia-Yu; Holbrook, Timothy R.; Calabrese, Federica; Wagner, Stephan; Zarejousheghani, Mashaalah; Griebe, Jan; Ullrich, Maria K.; Musat, Niculina; Schmidt, Matthias; Flyunt, Roman; Reemtsma, Thorsten; Richnow, Hans-Hermann; Stryhanyuk, Hryhoriy
    Nowadays, high-resolution imaging techniques are extensively applied in a complementary way to gain insights into complex phenomena. For a truly complementary analytical approach, a common sample carrier is required that is suitable for the different preparation methods necessary for each analytical technique. This sample carrier should be capable of accommodating diverse analytes and maintaining their pristine composition and arrangement during deposition and preparation. In this work, a new type of sample carrier consisting of a silicon wafer with a hydrophilic polymer coating was developed. The robustness of the polymer coating toward solvents was strengthened by cross-linking and stoving. Furthermore, a new method of UV-ozone cleaning was developed that enhances the adhesion of the polymer coating to the wafer and ensures reproducible surface-properties of the resulting sample carrier. The hydrophilicity of the sample carrier was recovered applying the new method of UV-ozone cleaning, while avoiding UV-induced damages to the polymer. Noncontact 3D optical profilometry and contact angle measurements were used to monitor the hydrophilicity of the coating. The hydrophilicity of the polymer coating ensures its spongelike behavior so that upon the deposition of an analyte suspension, the solvent and solutes are separated from the analyte by absorption into the polymer. This feature is essential to limit the coffee-ring effect and preserve the native identity of an analyte upon deposition. The suitability of the sample carrier for various sample types was tested using nanoparticles from suspension, bacterial cells, and tissue sections. To assess the homogeneity of the analyte distribution and preservation of sample integrity, optical and scanning electron microscopy, helium ion microscopy, laser ablation inductively coupled plasma mass spectrometry, and time-of-flight secondary ion mass spectrometry were used. This demonstrates the broad applicability of the newly developed sample carrier and its value for complementary imaging. © 2020 Author(s).