Article
Physics, Fluids & Plasmas
Michael A. Lam, Boris Khusid, Lou Kondic, William Meyer
Summary: The origins of glass transition in hard-sphere colloids remain elusive, and the cessation of long-time particle diffusivity does not suppress crystallization. Once a crystallite forms, its growth is controlled by particle diffusion in the depletion zone. The insight into the effect of vanishing particle mobility and particle sedimentation on crystallization will help engineer colloidal materials with controllable structure.
Article
Chemistry, Multidisciplinary
Willem Gispen, Gabriele M. Coli, Robin van Damme, C. Patrick Royall, Marjolein Dijkstra
Summary: Nucleation is crucial for crystal formation and is involved in various phenomena, yet many aspects of the nucleation process remain poorly understood. In this study, the excess of particles in a face-centered-cubic (fcc)-like environment compared to a hexagonal-close-packed (hcp)-like environment in a crystal nucleus of hard spheres is explained by the higher order structure in the fluid phase. Pentagonal bipyramids, known as inhibitors of crystal nucleation, transform into Siamese dodecahedra, which are closely similar to an fcc subunit, explaining the higher propensity for fcc growth in hard spheres. This crystallization and polymorph selection mechanism is generic for crystal nucleation from a dense, strongly correlated fluid phase.
Article
Chemistry, Physical
Ignacio Sanchez-Burgos, Eduardo Sanz, Carlos Vega, Jorge R. Espinosa
Summary: The computational characterization of polymorphic nucleation competition between face-centered cubic (fcc) and hexagonal-close packed (hcp) hard-sphere crystal phases was conducted, revealing that the hcp phase may have a slightly higher interfacial free energy than the fcc phase, leading to a decreased propensity to nucleate from the liquid. The abundance of each polymorph in grown crystals from different types of nuclei and the maintenance of polymorphic structure in post-critical crystals were also analyzed, providing insights into the intricate puzzle of colloidal hard-sphere crystallization.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Vivek Verma, Benjamin K. Hodnett
Summary: Pairs of polymorphs can be characterized by their equilibrium solubility ratios and interfacial energy ratios. Classical nucleation theory equations can predict the conditions in which metastable or stable polymorphs crystallize first. Domain diagrams have been developed based on the solubility ratios and interfacial energy ratios. The pre-exponential factor has a strong influence on expanding the kinetically metastable zone when the interfacial energies are low, but has little effect when the values are high. This study also identifies circumstances where a metastable polymorph with higher interfacial energy crystallizes first.
Article
Chemistry, Physical
Sahana Kale, Achim Lederer, Martin Oettel, Hans Joachim Schoepe
Summary: PMMA-PHSA particles have been used as a hard sphere model system since the 1980s. We investigate the fluid structure of fluorescent particles in three different solvents and compare them with analytical theory and computer simulations. The results show hard sphere behavior in decalin-TCE and charged sphere behavior in decalin-CHB and decalin-CHB-TBAB solvents, with reduced screening in the latter system compared to the bulk solvent.
Article
Chemistry, Physical
Adiran Garaizar, Tim Higginbotham, Ignacio Sanchez-Burgos, Andres R. Tejedor, Eduardo Sanz, Jorge R. Espinosa
Summary: Colloidal patchy particles with high-symmetry bonding were computationally studied, and the crystallization behavior was investigated. The competition of ordered phases and the nucleation mechanisms were found to be influenced by pressure and the structure of crystalline embryos.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Meng Wang, Jingkang Wang, Na Wang, Wenxi Song, Xin Huang, Ting Wang, Hongxun Hao
Summary: Nucleation, as a crucial process in crystallization, determines the physicochemical properties of crystal products. The mechanism of nucleation is not fully understood due to the complexity of molecular assembly. In this study, the connection between nucleation kinetics and solution chemistry was investigated using 3,5-dinitrobenzoic acid (DNBA) as a model compound. The existing form of DNBA molecules in solutions was analyzed, and the relationship between molecular existing form and nucleation kinetics was revealed. A possible nucleation mechanism of DNBA molecules in solution was proposed.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Chunhao Liu, Yongli Wang, Yihan Zhao, Xin Li, Na Wang, Xin Huang, Ting Wang, Hongxun Hao
Summary: The cooling crystallization behavior of flexible molecule chlorpropamide in four solvent systems was studied to understand the relationship between solution chemistry and polymorphic nucleation. The presence of dimers and solvated monomers in the solution was confirmed using online ATR-FTIR spectra. Molecular dynamics simulations and 2D nuclear overhauser effect spectroscopy revealed the molecular preassembled species in the solution. The self-association mode and conformational distribution of chlorpropamide in the solution were found to influence the nucleation process and polymorphic outcome.
CRYSTAL GROWTH & DESIGN
(2022)
Article
Chemistry, Multidisciplinary
Aina Semjonova, Agris Berzins
Summary: Concomitant crystallization of polymorphs is a significant issue for the pharmaceutical industry. The study investigated the use of crystallization additives to control crystallization and prevent the formation of multiple polymorphs simultaneously. The results demonstrated that certain additives can facilitate the formation of metastable forms and control the crystallization outcome of isonicotinamide (INA).
CRYSTAL GROWTH & DESIGN
(2023)
Article
Physics, Condensed Matter
J. Quentino, P. A. F. P. Moreira
Summary: This study utilized machine-learning systems to identify local structures in mono-component hard-sphere simulations and accurately distinguish solid and amorphous spheres.
EUROPEAN PHYSICAL JOURNAL B
(2021)
Article
Chemistry, Multidisciplinary
Jacob D. Zwilling, Xiao Jiang, Franklin Zambrano, Richard A. Venditti, Hasan Jameel, Orlin D. Velev, Orlando J. Rojas, Ronalds Gonzalez
Summary: Recent advances in developing sustainable, micro- and nanoscale materials from biobased resources have focused on utilizing lignin to strengthen the bioeconomy. However, there is a gap in the literature regarding the various interactions present during and after the formation of lignin micro- and nanoparticles (LPs). These interactions are influenced by the chemical composition, molecular weight distribution, and solvent/water polarity. Factors such as lignin concentration also play a role in nucleation and growth mechanisms, with LPs formed at low concentrations exhibiting larger particle sizes than those formed at higher concentrations.
Article
Chemistry, Multidisciplinary
Haoyu Peng, Ningning Tian, Changyou Yu, Ye Gao, Kangli Li, Hui Yan, Pengwei Zhao, Songgu Wu, Mingyang Chen, Junbo Gong
Summary: The experimental metastable zone widths of PE-DPE-H2O systems were measured using a polythermal method, and the nucleation behavior of PE and the influence of DPE on critical nucleus parameters were analyzed based on modified Sangwal's model and classical nucleation theory, respectively. The results show that dissolved DPE molecules can significantly affect the nucleation process.
CRYSTAL GROWTH & DESIGN
(2022)
Article
Mechanics
Yuan Lin, Ying Wang, Zixin Weng, Dingyi Pan, Jiawang Chen
Summary: The presence of bubbles in non-colloidal suspensions significantly affects the shear thinning behavior, with large bubbles enhancing shear thinning and nano-bubbles suppressing it. Additionally, nano-bubbles influence the particle organization behavior, leading to a larger critical strain for the finish of the organization process. Therefore, a degassing process is essential to obtain reliable rheological properties of the two-phase suspension system.
Review
Chemistry, Multidisciplinary
Shanshan Wu, Yi Chen, Xiaodong Guo, Yuzhou Wu
Summary: This review discusses the principles, processes, and applications of collagen mineralization in hard tissue repair, providing an important reference for studying the collagen biomineralization mechanism and applications in hard tissue regeneration and repair.
MATERIALS CHEMISTRY FRONTIERS
(2021)
Article
Environmental Sciences
Aleksandra Sander, Ana Petracic, Iva Zokic, Domagoj Vrsaljko
Summary: Biodiesel produced from waste feedstocks has a significant role in addressing climate change, waste disposal, and energy demand. Research on extractive deacidification with deep eutectic solvents provides valuable insights into the process, with experimental data and validation of a working hypothesis.
JOURNAL OF ENVIRONMENTAL MANAGEMENT
(2022)
Article
Biophysics
Ali Asghar Hakami Zanjani, Nicholas P. Reynolds, Afang Zhang, Tanja Schilling, Raffaele Mezzenga, Joshua T. Berryman
BIOPHYSICAL JOURNAL
(2020)
Article
Chemistry, Physical
Fabian Glatzel, Tanja Schilling
Summary: The dynamics of coarse-grained observables in systems out of thermal equilibrium can be described by the non-stationary generalized Langevin equation. This equation, originally derived for deterministic dynamics, is also applicable to stochastic processes. Therefore, methods for estimating and numerically propagating this equation can be used for data obtained in molecular dynamics simulations with stochastic thermostats or barostats.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Fabian Coupette, Long Zhang, Bjoern Kuttich, Andrei Chumakov, Stephan V. Roth, Lola Gonzalez-Garcia, Tobias Kraus, Tanja Schilling
Summary: We investigate network formation and percolation of carbon black using Monte Carlo simulations and experiments. The percolation threshold shows a quasi-universal relation with the weighted average radius of gyration of the aggregate ensemble. The concentration of large carbon black aggregates has a stronger influence on the percolation threshold than the concentration of small aggregates, while higher order moments of the size distribution do not affect the percolation threshold.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Physics, Multidisciplinary
Fabian Glatzel, Tanja Schilling
Summary: The underdamped, non-linear, generalized Langevin equation is widely used in modeling coarse-grained dynamics of soft and biological materials. This study highlights the importance of approximations in obtaining the equation from microscopic dynamics and discusses the implications on memory terms and fluctuation-dissipation relations. It shows that the commonly used structure with a potential of mean force, a linear memory term, and a related fluctuating force is not exact and cannot always be derived as a controlled approximation.
Article
Physics, Multidisciplinary
Wilkin Woehler, Tanja Schilling
Summary: This study investigates crystal nucleation in suspensions of hard spheres and finds that there is a significant discrepancy between experimentally observed nucleation rates and numerically computed rates at low supersaturations. By proposing an interpretation of the experimental data as a combination of nucleation and crystal growth processes, the long-standing dispute about the differing rates may be resolved.
PHYSICAL REVIEW LETTERS
(2022)
Review
Physics, Multidisciplinary
Tanja Schilling
Summary: This article discusses the construction of coarse-grained models for systems out of thermal equilibrium, including both equilibrium and non-equilibrium coarse-graining methods and numerical schemes.
PHYSICS REPORTS-REVIEW SECTION OF PHYSICS LETTERS
(2022)
Article
Chemistry, Physical
Christoph Widder, Fabian Koch, Tanja Schilling
Summary: In this paper, we present a numerical method to generate stochastic dynamics based on the generalized Langevin equation with a non-stationary memory kernel. By means of a projection operator formalism, this method allows us to coarse-grain a microscopic system with an explicitly time-dependent Liouvillian and reproduce the distributions of observables.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
P. Elsaesser, T. Schilling
Summary: We investigate the potential energy surface of anthracene, tetracene, and pentacene clusters consisting of up to 30 molecules. By applying the basin-hopping Monte Carlo algorithm, we successfully identify the lowest energy states of acene clusters. The acene molecules are modeled using the polymer-consistent force field-interface force field. The obtained structures with the lowest observed energy are presented, and the relative stability and accessibility of structures corresponding to local energy minima are discussed.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Joeri Opdam, Poshika Gandhi, Anja Kuhnhold, Tanja Schilling, Remco Tuinier
Summary: In this paper, we study excluded volume interactions, free volume fraction available, and phase behavior in mixtures of hard spheres and hard rods. Comparing the results of free volume theory and Monte Carlo simulations, we find that the novel approach predicts free volume and phase stability accurately.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Physics, Fluids & Plasmas
Fabian Coupette, Tanja Schilling
Summary: This study proposes a simple percolation criterion for solving various percolation problems, which can accurately calculate the percolation threshold for many solved problems. The criterion has a wide range of applicability, including random graphs, small-world networks, and percolation problems on various lattices. In addition, the study introduces a method to generate simple planar lattices with a prescribed percolation threshold.
Article
Physics, Fluids & Plasmas
Christoph Widder, Tanja Schilling
Summary: This study investigates the SIR model on directed graphs with heterogeneous transmission probabilities using the message-passing approximation. The research characterizes percolation transition, predicts cluster size distributions, and proposes vaccination strategies, comparing predictions to real network simulations. It is found that the predicted percolation threshold is a strict lower bound to the threshold on real networks, with good agreement between predictions and numerical data on large, locally treelike networks.
Article
Physics, Fluids & Plasmas
Fabian Coupette, Rene de Bruijn, Petrus Bult, Shari Finner, Mark A. Miller, Paul van der Schoot, Tanja Schilling
Summary: The study introduces a new method for estimating continuum percolation thresholds and demonstrates its usefulness through examples of geometric percolation. While the new method accurately predicts thresholds for slender nanofillers in three dimensions, it fails to do so in two dimensions, highlighting its stringency. Using simple geometric considerations, the method provides predictions that closely match Monte Carlo simulations, showcasing its effectiveness.
Article
Physics, Fluids & Plasmas
Hugues Meyer, Fabian Glatzel, Wilkin Woehler, Tanja Schilling
Summary: The study proposes to describe phase transition dynamics using a nonstationary generalized Langevin equation for the order parameter. It suggests that the extent of the memory kernel is positively correlated with the duration of the transition and is of the same order of magnitude, while the distribution of induction times does not affect the memory kernel. This observation is consistent with several model systems tested through computer simulations.
Article
Multidisciplinary Sciences
Hugues Meyer, Steffen Wolf, Gerhard Stock, Tanja Schilling
Summary: A method is presented to infer the memory kernel in non-equilibrium processes, using ion dissociation in water as an example. This method improves a previously published numerical scheme and addresses the issue of truncation.
ADVANCED THEORY AND SIMULATIONS
(2021)
Article
Physics, Fluids & Plasmas
M. Bueltmann, T. Schilling
