Article
Physics, Multidisciplinary
Tobias Eckert, Matthias Schmidt, Daniel de Las Heras
Summary: This study presents a theoretical approach based on sedimentation paths to predict the effect of gravity on sedimentation phases in mixtures of anisotropic colloids. By revisiting iconic sedimentation-diffusion-equilibrium experiments, the authors demonstrate how gravity and sample height can be control parameters to study bulk phase behavior.
COMMUNICATIONS PHYSICS
(2021)
Article
Chemistry, Physical
Nina Lorenz, Ishan Gupta, Thomas Palberg
Summary: We studied low-salt, binary aqueous suspensions of charged colloidal spheres with a size ratio of 0.57. The typical phase formed is a substitutional alloy with a body centered cubic structure. We also prepared the same samples using a different method which resulted in a complex sequence of gradients and a variety of microstructures. The observed crystallization processes are not volume-filling and the formed alloys are thermodynamically metastable without solid-fluid interfaces.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
J. Opdam, V. F. D. Peters, H. H. Wensink, R. Tuinier
Summary: A theoretical framework is proposed to quantify the thermodynamic properties of multicomponent hard colloidal mixtures. The phase behavior of mixtures of rods with spheres and rods with plates are predicted using this framework, taking into account the liquid crystal phases of both components. The study demonstrates a rich and complex range of phase behaviors, featuring a large variety of different multiphase coexistence regions. The approach can qualitatively account for certain multiphase equilibria observed in rod/plate mixtures and will be useful in tuning the phase behavior of shape-disperse mixtures in general.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Vincent F. D. Peters, Alvaro Gonzalez Garcia, Henricus H. Wensink, Mark Vis, Remco Tuinier
Summary: This study predicts the phase behavior of athermal rod-polymer mixtures using analytical equations of state for hard rod dispersions and free volume theory. It shows that various types of phase states can coexist depending on concentrations, rod aspect ratio, and polymer-rod size ratio, including novel two-, three-, and four-phase coexistences and isostructural coexistences. This work provides insight into conditions for particular multiphase coexistences in well-defined model colloidal rod-polymer mixtures.
Article
Physics, Fluids & Plasmas
Ryotaro Koshoji, Mitsuaki Kawamura, Masahiro Fukuda, Taisuke Ozaki
Summary: Through an unbiased random search approach, 12 putative densest binary sphere packings have been discovered, leading to an updated phase diagram. It was found that in the small radius range, multiple structures compete with each other for high packing fraction, achieved by introducing distortion or combining a few local dense structural units.
Article
Chemistry, Physical
Marjolein de Jager, Joris de Jong, Laura Filion
Summary: Computer simulations were used to study point defects in systems of soft colloidal particles, determining that the nature of lattice distortion is mainly determined by crystal structure. One-dimensional lattice distortions depend on dimensionality, with interstitial concentrations in BCC crystals reaching up to 1%.
Article
Physics, Fluids & Plasmas
Harukuni Ikeda, Kunimasa Miyazaki, Hajime Yoshino, Atushi Ikeda
Summary: By considering two-step replica symmetry breaking (2RSB), we extended the replica liquid theory to describe the multiple glass transitions of binary mixtures with large size disparities. In the large-dimension limit where mean-field theory becomes exact, our theory predicts three distinct glass phases when the size ratio of particles exceeds a critical value. These phases include the one-step replica symmetry breaking (1RSB) double glass, the 1RSB single glass, and the 2RSB double glass with a unique energy landscape topography.
Article
Chemistry, Multidisciplinary
Lijie Lei, Shuo Wang, Xuemao Zhou, Salah Eddine Ghellab, Guanhua Lin, Yongxiang Gao
Summary: The paper investigates mixtures of active and passive colloids through simulation and finds rich dynamic structures, including exclusion zone, yolk/shell cluster, and stable active-passive alloys to motile clusters. Different structures can be achieved by tuning various parameters.
FRONTIERS IN CHEMISTRY
(2022)
Article
Chemistry, Physical
J. Opdam, D. Guu, M. P. M. Schelling, D. G. A. L. Aarts, R. Tuinier, M. P. Lettinga
Summary: This study investigated the phase boundaries and interactions in aqueous mixtures containing colloidal rod-like fd-viruses and polystyrene spheres, revealing the importance of excluded volume interactions. Experimentally determined phase transitions showed good correspondence with theoretical predictions from free volume theory, highlighting the role of excluded volume of rod-like depletants in the system.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Elshadc Allahyarov, Hartmut Lowen, Alan R. Denton
Summary: In this study, we investigate the structural correlations in strongly asymmetric mixtures of binary charged colloids. We find that the amplitude of the big-small correlation peak is smaller than that of the big-big and small-small correlation peaks. Furthermore, we discover that an additional shifted Gaussian attractive potential between the small macroions is needed to accurately reproduce their correct pair correlations.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Rodrigo Braz Teixeira, Daniel de las Heras, Jose Maria Tavares, Margarida M. Telo da Gama
Summary: The phase behavior of a binary mixture of patchy particles is theoretically studied with consideration of the effects of size difference and gravity. It is found that the relative size of particles can be used to control the phase behavior of the mixture, with an increase in the size of one type of particles promoting mixing and potentially leading to changes in stacking sequences under gravity.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Physics, Fluids & Plasmas
Dingwen Qian, Monica Olvera de la Cruz
Summary: In this study, we investigate oppositely charged colloids with size and charge asymmetry under the influence of an external electric field. The large colloidal particles are connected by harmonic springs, arranging themselves into a hexagonal lattice, while the small particles demonstrate fluid-like motion without bonds. Our findings reveal that the system exhibits cluster formation with stable wave packets in the vibrations of the large particles when the external driving force exceeds a critical value.
Article
Chemistry, Physical
Thomas Zemb, Rose Rosenberg, Stjepan Marcelija, Dirk Haffke, Jean-Francois Dufreche, Werner Kunz, Dominik Horinek, Helmut Coelfen
Summary: The study demonstrates that giant critical fluctuations induced by weak centrifugal fields can be observed above the miscibility gap of a binary liquid mixture, causing gradients in ethanol concentration. The standard interpretation of sedimentation equilibrium in the analytical ultracentrifuge may yield incorrect results. The effects can be qualitatively understood and explained using the Flory-Huggins solution model coupled to density functional theory.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Wezi D. Mkandawire, Scott T. Milner
Summary: Predicting the mixing free energy of binary mixtures is challenging. This study presents a novel molecular dynamics simulation method to extract the chemical potential and interaction parameter for mixtures. The method is applied to benzene-pyridine mixtures and shows good agreement with other simulation methods, highlighting the importance of accurate potentials for representing mixture behavior.
Article
Chemistry, Physical
David Vorac, Philipp Maass, Artem Ryabov
Summary: This study investigates the impact of polydispersity on particle currents in single-file Brownian motion of hard spheres, revealing a recurring pattern in dependence of the hard-sphere diameters and mixing ratio. The behavior of particle currents can be inferred based on a basic unit cell in the two hard-sphere diameters space. The analysis explains the occurrence of pronounced maxima and minima of the currents and predicts their variation in the fully covered system limit.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Yogesh Shelke, Susana Marin -Aguilar, Fabrizio Camerin, Marjolein Dijkstra, Daniela J. Kraft
Summary: Colloidal molecules with anisotropic shapes and interactions have been utilized as model systems to understand the behavior of real molecules and develop materials with desired properties. By using electrostatic self-assembly, we have demonstrated that the shape of cubic particles plays a crucial role in achieving high yields of distinct colloidal molecules across a wide range of size ratios. Our protocol is not affected by the specific choice of colloidal particle material and can be extended to other templating particle shapes, significantly expanding the library of colloidal molecules that can be obtained with high yield and purity.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Letter
Chemistry, Multidisciplinary
Pauline J. Kolbeck, Mihir Dass, Irina V. Martynenko, Relinde J. A. van Dijk-Moes, Kelly J. H. Brouwer, Alfons van Blaaderen, Willem Vanderlinden, Tim Liedl, Jan Lipfert
Summary: Atomic force microscopy (AFM) is a powerful technique for high-resolution imaging of molecules, macromolecular complexes, and nanoparticles. However, the shape of the AFM tip can distort the images. In this study, we use a 3D DNA origami structure as a fiducial for tip reconstruction and image correction. The fiducial has sharp steps at different heights, allowing reliable tip reconstruction with as few as ten fiducials. This fiducial enables accurate and precise AFM imaging for a wide range of applications.
Article
Physics, Multidisciplinary
W. Q. Boon, M. Dijkstra, R. van Roij
Summary: Chemical reactions responsible for charging of solids in water are investigated theoretically, and it is found that the equilibration of surface charge contains important information on reaction mechanisms and ion valency. A nonlinear differential equation is constructed to describe surface charging by combining Langmuir kinetics and Poisson-Boltzmann theory. The relaxation rates at late-time and short-time reveal information on charge valency and ad- or desorption mechanism, and an inflection point during equilibration distinguishes single-ion reactions from two-ion reactions, suggesting a Coulombic ion-surface interaction as an autocatalytic feedback mechanism.
PHYSICAL REVIEW LETTERS
(2023)
Article
Chemistry, Physical
Nuno A. M. Araujo, Liesbeth M. C. Janssen, Thomas Barois, Guido Boffetta, Itai Cohen, Alessandro Corbetta, Olivier Dauchot, Marjolein Dijkstra, William M. Durham, Audrey Dussutour, Simon Garnier, Hanneke Gelderblom, Ramin Golestanian, Lucio Isa, Gijsje H. Koenderink, Hartmut Loewen, Ralf Metzler, Marco Polin, C. Patrick Royall, Andela Saric, Anupam Sengupta, Cecile Sykes, Vito Trianni, Idan Tuval, Nicolas Vogel, Julia M. Yeomans, Iker Zuriguel, Alvaro Marin, Giorgio Volpe
Summary: Self-organisation is the spontaneous emergence of spatio-temporal structures and patterns from the interaction of smaller individual units. Confinement can mediate and control self-organisation by limiting the translational and rotational degrees of freedom, acting as a catalyst or inhibitor. By constraining the self-organisation process in soft-matter systems, confinement can actively steer the emergence or suppression of collective phenomena in space and time.
Article
Multidisciplinary Sciences
Ramakrishna Kotni, Albert Grau-Carbonell, Massimiliano Chiappini, Marjolein Dijkstra, Alfons van Blaaderen
Summary: Liquid crystal phases are in-between solids and liquids, exhibiting long-range orientational order and flow properties, making them fundamental for optical applications. Researchers have discovered a previously elusive splay-bend nematic liquid crystal phase in a colloidal system of bent silica rods.
NATURE COMMUNICATIONS
(2022)
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
Yunhan Zhang, Giuliana Giunta, Haojun Liang, Marjolein Dijkstra
Summary: Leveraging the anisotropic shape of DNA-functionalized nanoparticles allows for shape-directed crystallization of various superlattice structures. Using molecular dynamics simulations, we observe the self-assembly of different phases (SC, pBCT, and d-pBCT) in a binary mixture of cubic gold nanoparticles functionalized with complementary DNA strands. We investigate the impact of DNA strand length, grafting density, and rigidity on the self-assembly behavior and find that longer and flexible DNA strands can induce a phase transformation from SC to pBCT due to increased entropy.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Albert Grau-Carbonell, Fabian Hagemans, Maarten Bransen, Nina A. Elbers, Relinde J. A. van Dijk-Moes, Sina Sadighikia, Tom A. J. Welling, Alfons van Blaaderen, Marijn A. van Huis
Summary: Researchers successfully determined the volume of PNIPAM microgels in water by labeling them and studied their thermoresponsive behavior and stability in water.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Computer Science, Artificial Intelligence
Simone Ciarella, Massimiliano Chiappini, Emanuele Boattini, Marjolein Dijkstra, Liesbeth M. C. Janssen
Summary: We present a machine-learning approach to predict the non-Markovian dynamics of supercooled liquids using static averaged quantities as input and output. Our method outperforms particle propensity-based techniques and is more applicable in experimental contexts where particle resolved information is not available. Our deep neural network can accurately predict the self intermediate scattering function of binary mixtures based on their static structure factor, and the model shows some transferability to lower temperatures or similar systems. Furthermore, we develop an evolutionary strategy that parameterizes the memory function of supercooled liquids as the sum of two stretched exponentials, corresponding to two dominant relaxation modes.
MACHINE LEARNING-SCIENCE AND TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Yogesh Shelke, Fabrizio Camerin, Susana Marin-Aguilar, Ruben W. Verweij, Marjolein Dijkstra, Daniela J. Kraft
Summary: In this study, flexible colloidal molecules with an in situ controllable motion range and bond directionality were created by assembling spherical particles onto cubes functionalized with complementary surface-mobile DNA. The size ratio of the sphere-to-cube varied to obtain colloidal molecules with different coordination numbers, and it was found that they exhibited a constrained range of motion above a critical size ratio. The confinement of the spheres on the surface of the cube and the probability to change facet were quantified, and temperature was identified as an extra control parameter to switch between full and constrained flexibility.
Article
Chemistry, Multidisciplinary
Aarya Prabhakaran, Zhiya Dang, Rohan Dhall, Fabrizio Camerin, Susana Marin-Aguilar, Balaji Dhanabalan, Andrea Castelli, Rosaria Brescia, Liberato Manna, Marjolein Dijkstra, Milena P. P. Arciniegas
Summary: Manipulating nano-objects through heating is an effective approach to modify the structure and optoelectronic properties of semiconducting materials. In this study, temperature-sensitive CsPbBr(3) perovskite nanoplatelets were synthesized and their structural evolution was observed at the nanoscale using in situ heating transmission electron microscopy. The morphological changes, starting from self-assembly into ribbons and ultimately forming randomly dispersed nanosheets on a substrate, were identified and supported by molecular dynamics simulations. The merging paths of the nanoplates within the ribbons were found to be influenced by the random orientation of the initial ribbons and the mobility of ligands, enabling the creation of structures with tunable emission ranging from blue to green.
Article
Chemistry, Multidisciplinary
Giuliana Giunta, Gerardo Campos-Villalobos, Marjolein Dijkstra
Summary: Colloidal nanoparticles can self-assemble into superstructures with distinctive properties. This study proposes a machine-learning approach to construct effective coarse-grained many-body interaction potentials for investigating the self-assembly behavior of complex colloidal systems. The key advantage of this method is its generality.
Article
Chemistry, Physical
Tor Sewring, Marjolein Dijkstra
Summary: Using Onsager-Straley's theory, this study investigates the cholesteric pitch of cellulose nanocrystal (CNC) suspensions. The research reveals that the twisting of chiral bundles significantly affects the helical twisting of the cholesteric phase. Moreover, the average particle length and length polydispersity have a substantial impact on strongly twisted bundles but minimal effects on weakly twisted ones.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Mark J. J. Mangnus, Vincent R. M. Benning, Bettina Baumgartner, P. Tim Prins, Thomas P. van Swieten, Ayla J. H. Dekker, Alfons van Blaaderen, Bert M. Weckhuysen, Andries Meijerink, Freddy T. Rabouw
Summary: This study investigates the influence of solvent and gas environments on the photoluminescence (PL) properties of lanthanide-doped nanocrystals, and explains the changes in PL spectrum and excited-state lifetimes using energy transfer mediated by molecular vibrations. EVET-mediated quenching holds promise for probing the local chemical environment of nanocrystals dispersed in a liquid or exposed to gaseous molecules.
Article
Chemistry, Multidisciplinary
Mark J. J. Mangnus, Vincent R. M. Benning, Bettina Baumgartner, P. Tim Prins, Thomas P. van Swieten, Ayla J. H. Dekker, Alfons van Blaaderen, Bert M. Weckhuysen, Andries Meijerink, Freddy T. Rabouw
Summary: The photoluminescence of lanthanide-doped nanocrystals can be quenched by energy transfer to nearby molecular vibrations, which is often undesired but can provide information about molecular vibrations in the local environment. This study investigates the influence of solvent and gas environments on the photoluminescence properties of NaYF4:Er3+,Yb3+ upconversion nanocrystals and relates the changes to quenching by electronic-to-vibrational energy transfer. The results suggest that EVET-mediated quenching can be used as a mechanism to probe the local chemical environment in liquid and gas-phase systems.
Article
Chemistry, Physical
Yiping Yin, Zhe Wang, Hua Zou
Summary: This study presents a novel method for preparing dimpled polymer-silica nanocomposite particles using interfacial swelling-based seeded polymerization. The optimized conditions allow for a relatively high percentage of dimpled particles to be achieved.
Article
Chemistry, Physical
Brenden D. Hoehn, Elizabeth A. Kellstedt, Marc A. Hillmyer
Summary: Porous materials with nanometer-scale pores have important applications as nanoporous membranes. In this study, ABA triblock copolymers were used as precursors to produce nanoporous polymeric membranes (NPMs) in thin film form by degrading the end blocks. Polycyclooctene (PCOE) NPMs with tunable pore sizes were successfully prepared using solvent casting technique. Oxygen plasma etching was employed to improve the surface porosity and hydrophilicity of the membranes. This study provides a straightforward method to produce tough NPMs with high porosity and hydrophilic surface properties.
Article
Chemistry, Physical
Vladislav S. Petrovskii, Stepan I. Zholudev, Igor I. Potemkin
Summary: This article investigates the behavior of linear and ring polypeptide chains in aqueous solution and explores the properties of the complexes formed by these chains with oppositely charged surfactants. The results demonstrate that the complexes of linear supercharged unfolded polypeptides and the corresponding surfactants exhibit impressive adhesive properties.
Article
Chemistry, Physical
Merve Cevik, Serkan Dikici
Summary: Cardiovascular diseases are a leading cause of death globally, and vascular grafts are a promising treatment option. This study focuses on tissue-engineered vascular grafts (TEVGs) using decellularized parsley stems as a potential biomaterial. The decellularized parsley stems showed suitable properties for TEVGs, providing a suitable environment for human endothelial cells to form a pseudo endothelium. This study showcases the potential of using parsley stems for TEVGs.
Article
Chemistry, Physical
Gustavo A. Vasquez-Montoya, Tadej Emersic, Noe Atzin, Antonio Tavera-Vazquez, Ali Mozaffari, Rui Zhang, Orlando Guzman, Alexey Snezhko, Paul F. Nealey, Juan J. de Pablo
Summary: The optical properties of liquid crystals are typically controlled by electric fields. In this study, we investigate the effects of microfluidic flows and acoustic fields on the molecular orientation and optical response of nematic liquid crystals. We identify several previously unknown structures and explain them through calculations and simulations. These findings hold promise for the development of new systems combining sound, flow, and confinement.
Article
Chemistry, Physical
Xinjun Wu, Xin Guan, Shushu Chen, Jiangpeng Jia, Chongyi Chen, Jiawei Zhang, Chuanzhuang Zhao
Summary: This research presents a novel shape memory hydrogel with a remodelable permanent shape and programmable cold-induced shape recovery behavior. The hydrogel is prepared using specific treatment methods to achieve shape fixation by heating and shape recovery by cooling. Additionally, deformable devices can be obtained by assembling hydrogel blocks with different concentrations.
Article
Chemistry, Physical
Rebecca Hengsbach, Gerhard Fink, Ulrich Simon
Summary: This study examines the properties of DNA functionalized pNipmam microgels and pure pNipmam microgels at different concentrations of sodium chloride and in PBS solutions using temperature dependent H-1-NMR measurements. The results show that DNA modification affects the volume phase transition temperature and the addition of salt and PBS further enhances this effect.
Article
Chemistry, Physical
Ningyi Li, Junhong Li, Lijingting Qing, Shicheng Ma, Yao Li, Baohui Li
Summary: This paper investigates the self-assembly behavior of colloids with competing interactions under spherical confinement and finds that different ordered structures can be formed under different sized spherical confinements. Moreover, more perforated structures are formed in smaller spheres.
