arXiv subjects

Jens Harting

Publications and source records attributed to Jens Harting.

At least 37 records · Page 2Linked to original sources

arXiv2025

Taxonomy of amorphous ternary phase diagrams: the importance of interaction parameters

Understanding phase diagrams is essential for material selection and design, as they provide a comprehensive representation of the thermodynamics of mixtures. This work delivers a broad and systematic overview of possible ternary phase diagrams for amorphous systems representative of polymers, small organic molecules, and solvents. Thanks to computationally efficient methods, an unprecedented library of $>$80,000 ternary phase diagrams is generated based on a systematic screening of interaction parameters. Twenty-one phase diagram types, including unreported ones, are identified. They are classified according to simple rules related to the number of immiscible material pairs, of miscibility gaps, and of three-phase regions. They are mapped onto the three-dimensional interaction parameters space, providing a clear picture of their likelihood and existence conditions. Four well-known phase-diagram types with 0, 1, 2, or 3 immiscible pairs are found to be the most likely. The numerous uncommon phase diagrams are mostly observed within a small parameter window around the critical interaction parameter values. For the most common phase diagram types, we show that the size of the processability window becomes sensitive to interaction parameter variations close to critical values. The sensitivity decreases for materials with increasing molar size. Finally, successful comparisons of simulated and experimental phase diagrams showcase the real-world relevance of this theoretical analysis. The presented results lay a robust foundation for rational design of solution processing conditions and for blend morphology control. Immediate applications include organic thin films and the identification of green solvents for sustainable processing.

cond-mat.mtrl-sci↗

arXiv2024

Reaction-limited evaporation for the color-gradient lattice Boltzmann model

We present a method to achieve reaction-limited evaporation for the color-gradient lattice Boltzmann multicomponent model. Our approach involves a systematic way to remove fluid mass from the interface region in order to achieve evaporation rates similar to those in a reaction-limited regime. Through various tests, our method demonstrates accurate and consistent results for different interface shapes across a wide range of evaporation flux magnitudes. A single free parameter is required to choose the evaporation sites where fluid mass is exchanged between the components. We find that at unit density ratio, this single parameter allows for the correct description of an arbitrarily shaped interface with an error of less than 5%. For density contrasts, accurate results are observed for lower evaporation flux magnitudes and density ratios. Our proposed method can be applied to isothermal reaction-limited scenarios, such as evaporation in pure vapor or under a gas draft. It can also handle weakly space-time-dependent fluxes, making it suitable for specific non-isothermal applications such as drop evaporation from heated substrates.

physics.flu-dyn↗

arXiv2024

Phase field simulations of thermal annealing for all-small molecule organic solar cells

Interest in organic solar cells (OSCs) is constantly rising in the field of photovoltaic devices. The device performance relies on the bulk heterojunction (BHJ) nanomorphology, which develops during the drying process and additional post-treatment. This work studies the effect of thermal annealing (TA) on an all-small molecule DRCN5T: PC71 BM blend with phase field simulations. The objective is to determine the physical phenomena driving the evolution of the BHJ morphology for a better understanding of the posttreatment/morphology relationship. Phase-field simulation results are used to investigate the impact on the final BHJ morphology of the DRCN5T crystallization-related mechanisms, including nucleation, growth, crystal stability, impingement, grain coarsening, and Ostwald ripening, of the amorphous-amorphous phase separation (AAPS), and of diffusion limitations. The comparison of simulation results with experimental data shows that the morphological evolution of the BHJ under TA is dominated by dissolution of the smallest, unstable DRCN5T crystals and anisotropic growth of the largest crystals.

cond-mat.mtrl-sci↗

arXiv2024

Modeling of thin liquid films with arbitrary many layers

We propose the generalization of the thin film equation (TFE) to arbitrarily many immiscible liquid layers. Then, we provide different pathways for deriving the hydrodynamic pressure within the individual layers, showing how to understand the equation as a Cahn-Hilliard-type conservation equation and providing an algorithm to derive the associated Onsager Matrix. Furthermore, we employ a numerical solver based on the multilayer shallow water-lattice Boltzmann method (LBM) for two and three liquid layers in pseudo two and three dimensions to gain insights into the dynamics of the system and to validate the model. We perform a linear stability analysis and assess droplet equilibrium shapes. Furthermore, we compare the dynamics of the proposed thin film equation to full Navier-Stokes simulations and show the possible equilibrium states of the multilayer liquid thin film system.

physics.flu-dyn↗

arXiv2024

Margination of artificially stiffened red blood cells

Margination, a fundamental process in which leukocytes migrate from the flowing blood to the vessel wall, is well-documented in physiology. However, it is still an open question on how the differences in cell size and stiffness of white and red cells contribute to this phenomenon. To investigate the specific influence of cell stiffness, we conduct experimental and numerical studies on the segregation of a binary mixture of artificially stiffened red blood cells within a suspension of healthy cells. The resulting distribution of stiffened cells within the channel is found to depend on the channel geometry, as demonstrated with slit, rectangular, and cylindrical cross-sections. Notably, an unexpected central peak in the distribution of stiffened RBCs, accompanied by fourfold peaks at the corners, emerges in agreement with simulations. Our results unveil a non-monotonic variation in segregation/margination concerning hematocrit and flow rate, challenging the prevailing belief that higher flow rates lead to enhanced margination.

cond-mat.soft↗

arXiv2024

Towards a universal law for blood flow

Despite decades of research on blood flow, an analogue of Navier-Stokes equations that accurately describe blood flow properties has not been established yet. The reason behind this is that the properties of blood flow seem à priori non universal as they depend on various factors such as global concentration of red blood cells (RBCs) and channel width. Here, we have discovered a universal law when the stress and strain rate are measured at a given local RBCs concentration. However, the local concentration must be determined in order to close the problem. We propose a non-local diffusion equation of RBCs concentration that agrees with the full simulation. The universal law is exemplified for both shear and pressure driven flows. While the theory is restricted to a simplistic geometry (straight channel) it provides a fundamental basis for future research on blood flow dynamics and could lead to the development of a new theory that accurately describes blood flow properties under various conditions, such as in complex vascular networks.

physics.flu-dyn↗

arXiv2024

Self-assembled porous media from particle-stabilized emulsions

We propose a new mechanism to create self-assembled porous media with highly tunable geometrical properties and permeabilities: We first allow a particle-stabilized emulsion to form from a mixture of two fluids and colloidal particles. Then, either one fluid phase or the particle layer is solidified, which can be achieved by techniques such as polymerization or freezing. Based on computer simulations we demonstrate that modifying only the particle wettability or concentration results in porous structures with a wide range of pore sizes and a permeability that can be varied by up to three orders of magnitude. We then discuss optimization of these properties for self-assembled filters or reactors and conclude that structures based on so-called "bijels" are most suitable candidates.

cond-mat.soft↗

arXiv2024

Enhancement of bubble transport in porous electrodes and catalysts

We investigate the formation and transport of gas bubbles across a model porous catalyst/electrode using lattice Boltzmann simulations. This approach enables us to systematically examine the influence of a wide range of morphologies, flow velocities, and reaction rates on the efficiency of gas production. By exploring these parameters, we identify critical parameter combinations that significantly contribute to an enhanced yield of gas output. Our simulations reveal the existence of an optimal pore geometry for which the product output is maximized. Intriguingly, we also observe that lower flow velocities improve gas production by leveraging on coalescence-induced bubble detachment from the catalyst.

cond-mat.soft↗

arXiv2024

Chemically reactive thin films: dynamics and stability

Catalyst particles or complexes suspended in liquid films can trigger chemical reactions leading to inhomogeneous concentrations of reactants and products in the film. We demonstrate that the sensitivity of the liquid film's gas-liquid surface tension to these inhomogeneous concentrations strongly impacts the film stability. Using linear stability analysis, we identify novel scenarios in which the film can be either stabilized or destabilized by the reactions. Furthermore, we find so far unrevealed rupture mechanisms which are absent in the chemically inactive case. The linear stability predictions are confirmed by numerical simulations, which also demonstrate that the shape of chemically active droplets can depart from the spherical cap and that unsteady states such as traveling and standing waves might appear. Finally, we critically discuss the relevance of our predictions by showing that the range of our selected parameters is well accessible by typical experiments.

cond-mat.soft↗

arXiv2023

Crystalline Morphology Formation in Phase-Field Simulations of Binary Mixtures

Understanding the morphology formation process of solution-cast photoactive layers (PALs) is crucial to derive design rules for optimized and reliable third generation solar cell fabrication. For this purpose, a Phase-Field (PF) computational framework dedicated to the simulation of PAL processing has recently been developed. In this study focused on non-evaporating, crystallizing binary mixtures, distinct crystalline morphology formation pathways are characterized by a systematic exploration of the model's parameter space. It is identified how, depending on material properties, regular, dilution-enhanced, diffusion-limited and demixing-assisted crystallization can take place, and which associated structures then arise. A comprehensive description of the thermodynamic and kinetic mechanisms that respectively drive these separate crystallization modes is provided. Finally, comparisons with experimental results reported in the literature highlight the promising potential of PF simulations to support the determination of process-structure relationships for improved PAL production.

cond-mat.mtrl-sci↗

arXiv2023

A sharp interface approach for wetting dynamics of coated droplets and soft particles

The wetting dynamics of liquid particles, from coated droplets to soft capsules, holds significant technological interest. Motivated by the need to simulate liquid metal droplet with an oxidize surface layer, in this work we introduce a computational scheme that allows to simulate droplet dynamics with general surface properties and model different levels of interface stiffness, describing also cases that are intermediate between pure droplets and capsules. Our approach is based on a combination of the immersed boundary (IB) and the lattice Boltzmann (LB) methods. Here, we validate our approach against the theoretical predictions in the context of shear flow and static wetting properties and we show its effectiveness in accessing the wetting dynamics, exploring the ability of the scheme to address a broad phenomenology.

physics.flu-dyn↗

arXiv2023

Suspensions of viscoelastic capsules: effect of membrane viscosity on transient dynamics

Membrane viscosity is known to play a central role in the transient dynamics of isolated viscoelastic capsules by decreasing their deformation, inducing shape oscillations and reducing the loading time, that is, the time required to reach the steady-state deformation. However, for dense suspensions of capsules, our understanding of the influence of the membrane viscosity is minimal. In this work, we perform a systematic numerical investigation based on coupled immersed boundary -- lattice Boltzmann (IB-LB) simulations of viscoelastic spherical capsule suspensions in the non-inertial regime. We show the effect of the membrane viscosity on the transient dynamics as a function of volume fraction and capillary number. Our results indicate that the influence of membrane viscosity on both deformation and loading time strongly depends on the volume fraction in a non-trivial manner: dense suspensions with large surface viscosity are more resistant to deformation but attain loading times that are characteristic of capsules with no surface viscosity, thus opening the possibility to obtain richer combinations of mechanical features.

cond-mat.soft↗

arXiv2023

Viscous to inertial coalescence of liquid lenses: a lattice Boltzmann investigation

Liquid lens coalescence is an important mechanism involved in many industrial and scientific applications. It has been investigated both theoretically and experimentally, yet it is numerically very challenging to obtain consistent results over the wide ranges of surface tension and viscosity values that are necessary to capture the asymptotic temporal behavior in the viscous and inertial limits. We report results of massively parallel simulations based on the color gradient lattice Boltzmann method, which overcome these limitations, and investigate the scaling laws of both regimes. For the two-dimensional case we find good agreement with the similarity solution of the thin-sheet equation, where in the viscous regime the connecting bridge grows linearly with time and in the inertial regime proportionally to $t^{2/3}$. In three dimensions, the viscous growth of the bridge also exhibits a linear time dependence, while in the inertial regime the growth of both the bridge height and the bridge width is proportional to $t^{1/2}$.

physics.flu-dyn↗

arXiv2023

Cell-free layer development and spatial organization of healthy and rigid red blood cells in a microfluidic bifurcation

Bifurcations and branches in the microcirculation dramatically affect blood flow as they determine the spatiotemporal organization of red blood cells (RBCs). Such changes in vessel geometries can further influence the formation of a cell-free layer (CFL) close to the vessel walls. Biophysical cell properties, such as their deformability, which is impaired in various diseases, are often thought to impact blood flow and affect the distribution of flowing RBCs. This study investigates the flow behavior of healthy and artificially hardened RBCs in a bifurcating microfluidic T-junction. We determine the RBC distribution across the channel width at multiple positions before and after the bifurcation. Thus, we reveal distinct focusing profiles in the feeding mother channel for rigid and healthy RBCs that dramatically impact the cell organization in the successive daughter channels. Moreover, we experimentally show how the characteristic asymmetric CFLs in the daughter vessels develop along their flow direction. Complimentary numerical simulations indicate that the buildup of the CFL is faster for healthy than for rigid RBCs. Our results provide fundamental knowledge to understand the partitioning of rigid RBC as a model of cells with pathologically impaired deformability in complex in vitro networks.

physics.bio-ph↗

arXiv2022

Modelling diffusive transport of particles interacting with slit nanopore walls: The case of fullerenes in toluene filled alumina pores

Accurate modeling of diffusive transport of nanoparticles across nanopores is a particularly challenging problem. The reason is that for such narrow pores the large surface-to-volume ratio amplifies the relevance of the nanoscopic details and of the effective interactions at the interface with pore walls. Close to the pore wall, there is no clear separation between the length scales associated with molecular interactions, layering of the solvent at the interface with the pore and the particle size. Therefore, the standard hydrodynamic arguments may not apply and alternative solutions to determining average transport coefficients need to be developed. We here address this problem by offering a multiscale ansatz that uses effective potentials determined from molecular dynamics simulations to parametrise a four state stochastic model for the positional configuration of the particle in the pore. This is in turn combined with diffusivities in the centre of the pore and at the pore wall to calculate the average diffusion constant. We apply this model to the diffusion of fullerenes in a toluene filled slit nanopore and calculate the mean diffusion coefficient as a function of the pore size. We show that the accuracy of our model is affected by the partial slip of the toluene on the pore wall.

cond-mat.mes-hall↗

arXiv2022

Formation of crystalline bulk heterojunctions in organic solar cells: insights from phase-field simulations

The performance of organic solar cells strongly depends on the bulk heterojunction (BHJ) morphology of the photoactive layer. This BHJ forms during the drying of the wet-deposited solution, because of physical processes such as crystallization and/or liquid liquid phase separation (LLPS). However, the process-structure relationship remains insufficiently understood. In this work, a recently developed, coupled phase field fluid mechanics framework is used to simulate the BHJ formation upon drying. For the first time, this allows to investigate the interplay between all the relevant physical processes (evaporation, crystal nucleation and growth, liquid demixing, composition-dependent kinetic properties), within a single coherent theoretical framework. Simulations for the model system P3HT-PCBM are presented. The comparison with previously reported in-situ characterization of the drying structure is very convincing: the morphology formation pathways, crystallization kinetics, and final morphology are in line with experimental results. The final BHJ morphology is a subtle mixture of pure crystalline donor and acceptor phases, pure and mixed amorphous domains, which depends on the process parameters and material properties. The expected benefit of such an approach is to identify physical design rules for ink formulation and processing conditions to optimize the cell performance. It could be applied to recent organic material systems in the future.

cond-mat.mtrl-sci↗

arXiv2022

Inertial focusing of a dilute suspension in pipe flow

The dynamics of rigid particle suspensions in a wall-bounded laminar flow present several non-trivial and intriguing features, including particle ordering, lateral transport, and the appearance of stable, preferential locations like the Segré-Silberberg annulus. The formation of more than one annulus is a particularly puzzling phenomenon that is still not fully explained. Here, we present numerical simulation results of a dilute suspension of particles in (periodic) pipe flow based on the lattice Boltzmann and the discrete element methods (DEM). Our simulations provide access to the full radial position history of the particles while traveling downstream. This allows to accurately quantify the transient and steady states. We observe the formation of the secondary, inner annulus and show that its position invariably shifts toward the Segré-Silberberg one if the channel is sufficiently long, proving that it is, in fact, a transient feature for Reynolds numbers (Re) up to 600. We quantify the variation of the channel focusing length ($L_s/2R$) with Re. Interestingly and unlike the theoretical prediction for a point-like particle, we observe that $L_s/2R$ increases with Re for both the single particle and the suspension.

physics.flu-dyn↗

arXiv2022

Phase-field simulations of the morphology formation in evaporating crystalline multicomponent films

In numerous solution-processed thin films, a complex morphology resulting from liquid-liquid phase separation (LLPS) or from polycrystallization arises during the drying or subsequent processing steps. The morphology has a strong influence on the performance of the final device but unfortunately the process-structure relationship is often poorly and only qualitatively understood. This is because many different physical mechanisms (miscibility, evaporation, crystallization, diffusion, advection) are active at potentially different time scales, and because the kinetics plays a crucial role: the morphology develops until it is kinetically quenched far from equilibrium. In order to unravel the various possible structure formation pathways, we propose a unified theoretical framework that takes into account all these physical phenomena. This phase-field simulation tool is based on the Cahn-Hilliard equations for diffusion and the Allen-Cahn equation for crystallization and evaporation, which are coupled to the equations for the dynamics of the fluid. We discuss and verify the behavior of the coupled model based on simple test cases. Furthermore, we illustrate how this framework allows to investigate the morphology formation in a drying film undergoing evaporation-induced LLPS and crystallization, which is typically a situation encountered, e.g., in organic photovoltaics applications.

physics.app-ph↗