Universität Stuttgart

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Institute: search.filters.UBSInstitut.Institut für ComputerphysikInstitute: search.filters.UBSInstitut.Max-Planck-Institut für Intelligente Systeme

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    Ionic liquids in conducting nanoslits : how important is the range of the screened electrostatic interactions?
    (2022) Groda, Yaroslav; Dudka, Maxym; Oshanin, Gleb; Kornyshev, Alexei A.; Kondrat, Svyatoslav
    Analytical models for capacitive energy storage in nanopores attract growing interest as they can provide in-depth analytical insights into charging mechanisms. So far, such approaches have been limited to models with nearest-neighbor interactions. This assumption is seemingly justified due to a strong screening of inter-ionic interactions in narrow conducting pores. However, how important is the extent of these interactions? Does it affect the energy storage and phase behavior of confined ionic liquids? Herein, we address these questions using a two-dimensional lattice model with next-nearest and further neighbor interactions developed to describe ionic liquids in conducting slit confinements. With simulations and analytical calculations, we find that next-nearest interactions enhance capacitance and stored energy densities and may considerably affect the phase behavior. In particular, in some range of voltages, we reveal the emergence of large-scale mesophases that have not been reported before but may play an important role in energy storage.
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    A complementary experimental and theoretical approach for probing the surface functionalization of ZnO with molecular catalyst linkers
    (2023) Kousik, Shravan R.; Solodenko, Helena; YazdanYar, Azade; Kirchhof, Manuel; Schützendübe, Peter; Richter, Gunther; Laschat, Sabine; Fyta, Maria; Schmitz, Guido; Bill, Joachim; Atanasova, Petia
    The application of ZnO materials as solid-state supports for molecular heterogeneous catalysis is contingent on the functionalization of the ZnO surface with stable self-assembled monolayers (SAMs) of catalyst linker molecules. Herein, experimental and theoretical methods are used to study SAMs of azide-terminated molecular catalyst linkers with two different anchor groups (silane and thiol) on poly and monocrystalline (0001, ) ZnO surfaces. Angle-resolved and temperature-dependent X-ray photoelectron spectroscopy (XPS) is used to study SAM binding modes, thermal stabilities, and coverages. The binding strengths and atomistic ordering of the SAMs are determined via atom-probe tomography (APT). Density functional theory (DFT) and ab initio molecular dynamics (AIMD) calculations provide insights on the influence of the ZnO surface polarity on the interaction affinity and conformational behavior of the SAMs. The investigations show that SAMs based on 3-azidopropyltriethoxysilane possess a higher binding strength and thermal stability than the corresponding thiol. SAM surface coverage is strongly influenced by the surface polarity of ZnO, and the highest coverage is observed on the polycrystalline surface. To demonstrate the applicability of linker-modified polycrystalline ZnO as a catalyst support, a chiral Rh diene complex is immobilized on the azide-terminal of the SAM and its coverage is evaluated via XPS.
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    How to speed up ion transport in nanopores
    (2020) Breitsprecher, Konrad; Janssen, Mathijs; Srimuk, Pattarachai; Mehdi, B. Layla; Presser, Volker; Holm, Christian; Kondrat, Svyatoslav
    Electrolyte-filled subnanometre pores exhibit exciting physics and play an increasingly important role in science and technology. In supercapacitors, for instance, ultranarrow pores provide excellent capacitive characteristics. However, ions experience difficulties in entering and leaving such pores, which slows down charging and discharging processes. In an earlier work we showed for a simple model that a slow voltage sweep charges ultranarrow pores quicker than an abrupt voltage step. A slowly applied voltage avoids ionic clogging and co-ion trapping - a problem known to occur when the applied potential is varied too quickly - causing sluggish dynamics. Herein, we verify this finding experimentally. Guided by theoretical considerations, we also develop a non-linear voltage sweep and demonstrate, with molecular dynamics simulations, that it can charge a nanopore even faster than the corresponding optimized linear sweep. For discharging we find, with simulations and in experiments, that if we reverse the applied potential and then sweep it to zero, the pores lose their charge much quicker than they do for a short-circuited discharge over their internal resistance. Our findings open up opportunities to greatly accelerate charging and discharging of subnanometre pores without compromising the capacitive characteristics, improving their importance for energy storage, capacitive deionization, and electrochemical heat harvesting.
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    Nanoalignment by critical Casimir torques
    (2024) Wang, Gan; Nowakowski, Piotr; Farahmand Bafi, Nima; Midtvedt, Benjamin; Schmidt, Falko; Callegari, Agnese; Verre, Ruggero; Käll, Mikael; Dietrich, Siegfried; Kondrat, Svyatoslav; Volpe, Giovanni
    The manipulation of microscopic objects requires precise and controllable forces and torques. Recent advances have led to the use of critical Casimir forces as a powerful tool, which can be finely tuned through the temperature of the environment and the chemical properties of the involved objects. For example, these forces have been used to self-organize ensembles of particles and to counteract stiction caused by Casimir-Liftshitz forces. However, until now, the potential of critical Casimir torques has been largely unexplored. Here, we demonstrate that critical Casimir torques can efficiently control the alignment of microscopic objects on nanopatterned substrates. We show experimentally and corroborate with theoretical calculations and Monte Carlo simulations that circular patterns on a substrate can stabilize the position and orientation of microscopic disks. By making the patterns elliptical, such microdisks can be subject to a torque which flips them upright while simultaneously allowing for more accurate control of the microdisk position. More complex patterns can selectively trap 2D-chiral particles and generate particle motion similar to non-equilibrium Brownian ratchets. These findings provide new opportunities for nanotechnological applications requiring precise positioning and orientation of microscopic objects.
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    Manipulating wetting and pore filling by wall transparency
    (2025) Kondrat, Svyatoslav; Schimmele, Lothar; Giacomello, Alberto; Tasinkevych, Mykola; Dietrich, S.
    Atomically thin walls become increasingly prevalent in modern technologies. Exhibiting a unique property-transparency to interparticle interactions-such walls influence processes as diverse as capacitive energy storage, electron transfer, and wetting. However, the impact of wall transparency on wetting and capillary phenomena remains poorly understood. Herein, we employ classical density functional theory to explore how van der Waals interactions across thin solid walls affect capillarity and substrate wetting. Our findings demonstrate that a fluid-filled, sidewise-open channel beneath a thin wall can drastically enhance the lyophobicity of the wall (hydrophobicity if fluid is water), up to the point of effectively transforming lyophilic surfaces into lyophobic ones. Conversely, a fluid covering a thin wall can convert capillary condensation to drying and induce unusual capillary phases within the channel. These findings highlight the potential of wall transparency as a tool for manipulating channel filling and wetting behaviors, emphasizing its significance for interfacial phenomena and fluid adsorption in porous materials.