Article
Chemistry, Physical
Kazem V. Edmond, Tess W. P. Jacobson, Joon Suk Oh, Gi-Ra Yi, Andrew D. Hollingsworth, Stefano Sacanna, David J. Pine
Summary: This method involves the large-scale fabrication of bowl-shaped colloidal particles using an emulsion templating technique, where compliant seed particles are deformed by surface tension on oil droplets as templating surfaces. By adjusting droplet size and seed particle diameter, the final particle shape can be precisely controlled, ranging from shallow lenses to deep bowls. The resulting uniformly-shaped colloidal particles allow for depletion-mediated assembly of flexible colloidal chains and clusters.
Article
Chemistry, Physical
Wei Li, Kris T. Delaney, Glenn H. Fredrickson
Summary: The study developed a SCFT method to investigate polymer-mediated colloidal interactions, focusing on depletion effects and exploring mean-field interactions under different physical conditions. The results demonstrated good agreement with previous studies and experiments, extending the work to new regimes and discussing the mechanisms of attraction and repulsion along with the influence of individual factors.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Wenling Guo, Yulong He, Fawei Wang, Yonggang Li, Bin Wang, Rongmin Wang, Pengfei Song
Summary: A novel thin-wall bowl-shaped particles (BSPs) were prepared using the solvent-induced phase separation method, with Ag nanoparticles (AgNPs) loaded on the surface for excellent antibacterial properties against E. coli and S. aureus. This has promising application prospects in the prevention and treatment of bacterial infections.
COLLOID AND INTERFACE SCIENCE COMMUNICATIONS
(2021)
Article
Multidisciplinary Sciences
Zhe Xu, Theodore Hueckel, William T. M. Irvine, Stefano Sacanna
Summary: The research team has created non-biological capsules that can capture, concentrate, store, and release microscopic payloads as needed. This design uses hollow colloids as cell-membrane mimics with a well-defined single pore, allowing for mass production and offering a blueprint for developing smart materials, micro-machinery, and artificial cell mimics.
Article
Chemistry, Multidisciplinary
Xia Yin, Jing Yang, Mengji Zhang, Xinyao Wang, Wei Xu, Cameron-Alexander H. Price, Lin Huang, Wanshan Liu, Haiyang Su, Wenjing Wang, Hongyu Chen, Guangjin Hou, Mark Walker, Ying Zhou, Zhen Shen, Jian Liu, Kun Qian, Wen Di
Summary: Chemotherapy is a crucial cancer treatment, and its monitoring plays a vital role in improving survival rates and quality of life for cancer patients. However, current monitoring methods are not sensitive enough and have radiation invasiveness. In this study, a bowl-shaped submicroreactor chip loaded with Au-3-aminophenol formaldehyde resin (APF-bowl&Au) is developed for serum metabolic fingerprint extraction and chemotherapy monitoring, allowing for improved prediction of chemotherapy outcomes.
Review
Chemistry, Physical
Marjolein Dijkstra, Erik Luijten
Summary: This review provides an overview of computational tools and strategies used for the design of soft materials created through self-assembly of colloids and nanoparticles, including simulation methods, machine learning, and reverse-engineering. These tools are essential for guiding experimental synthesis efforts and offer new paradigms for understanding and predicting novel colloidal materials.
Article
Chemistry, Physical
Rachel S. Hendley, Lechuan Zhang, Michael A. Bevan
Summary: This study demonstrates the assembly of different shaped colloidal particles into ordered microstructures using a two-dimensional AC electric field. By controlling particle shape and field conditions, various liquid crystal structures and crystals can be assembled. These findings provide design rules for the assembly of diverse microstructures in AC electric fields and could have implications for particle-based materials, display technologies, and printing technologies.
Article
Polymer Science
Fei Xu, Wenhua Jing, Gaojian Chen, Zexin Zhang
Summary: The study presents a simple and effective method for synthesizing composite bowl-shaped colloidal particles, with bowl-shape determined by stirring and centrifugal force. Bowl size, thickness, and functional groups can be tuned by varying stirring speed, TPM monomer amount, and adding initiators and functional monomers during synthesis. The resulting particles exhibit biological activity and can be further modified to produce micromotors with controlled motions.
Article
Multidisciplinary Sciences
Lucia Baldauf, Erin G. Teich, Peter Schall, Greg van Anders, Laura Rossi
Summary: Creating materials with independently controllable structures at multiple scales requires breaking naturally occurring hierarchies. This study demonstrates that shape and interaction decoupling can occur in colloidal cuboids, leading to the formation of preassembled mesoscale building blocks for larger-scale structures. The results highlight the potential of preassembled building blocks for hierarchical materials design.
Article
Chemistry, Multidisciplinary
Jorge Sanchez Llorens, Lorenzo Barbera, Ahmet F. Demirors, Andre R. Studart
Summary: A light-based printing platform is reported to shape colloidal glasses into 3D objects with complex geometries and vivid structural color. The photonic properties of the printed objects reflect the locally ordered microstructure of the glass. The platform demonstrates the capability to create 3D objects with isotropic structural color.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Michael P. Howard, Zachary M. Sherman, Adithya N. Sreenivasan, Stephanie A. Valenzuela, Eric V. Anslyn, Delia J. Milliron, Thomas M. Truskett
Summary: This study demonstrates that the flexibility of the linker plays a key role in determining the phase behavior and structure of the colloid-linker mixture. Different flexibilities of the linker lead to different mixture behaviors, with flexible and rigid linker mixtures phase-separating at low colloid volume fractions, while semiflexible linker mixtures do not. The flexibility of the linker also influences the spacing between linked colloids, suggesting strategies for designing gels with desired properties.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Multidisciplinary Sciences
Mohammad Nabizadeh, Safa Jamali
Summary: The study explores the coupling between the kinetics of colloidal bonds and rheological response in attractive gels under different flow regimes. It reveals the importance of interplay between particle attraction and hydrodynamic stresses in understanding the physical basis of colloidal gel rheology. The research also presents visual mapping of particle bond dynamics and stresses under various flow conditions.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Xian Qi, Yaxian Du, Ziqiang Zhang, Xu Zhang
Summary: Janus particles for oil-water separation have been widely studied. In this study, bowl-shaped Janus particles were prepared using a thiol-ene click reaction and selective etching. These particles showed convex hydrophilic and concave oleophilic surfaces and exhibited high efficiency in separating micro-sized oil droplets from an emulsion within a short period of time. The underlying mechanism for the coalescence of oil droplets using these Janus particles was proposed based on experimental and theoretical results.
Article
Mechanics
Alessandro Patti, Alejandro Cuetos
Summary: Understanding the behavior of colloidal suspensions in confined environments is crucial for practical applications. By studying how colloids behave in nanopores, it is possible to control their phase behavior and stabilize unique morphologies that cannot form in bulk. The dynamics of colloids in confined environments are significantly influenced by their ability to diffuse in different directions within the nanopores.
Article
Chemistry, Physical
Thomas G. Mason
Summary: This study extends the concept of depletion forces between spheres to depletion torques affecting the orientations of colloidal particles with complex shapes. It demonstrates that depletion torques can be tailored by designing specific geometrical features in the shapes of particles.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Massimiliano Chiappini, Simone Dussi, Bruno Frka-Petesic, Silvia Vignolini, Marjolein Dijkstra
Summary: In this study, a simple model was used to describe cellulose nanocrystals (CNCs) and predict their pitch. The results suggest that the shape of the bundles can induce a chiral interaction between CNCs, explaining how chirality is transferred from the molecular scale to the cholesteric order.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Multidisciplinary Sciences
Gabriele M. Coli, Emanuele Boattini, Laura Filion, Marjolein Dijkstra
Summary: Colloidal self-assembly is a key method for producing next-generation materials, but the vast variety of colloidal building blocks and thermodynamic conditions make systematic exploration difficult. This study presents a generic inverse design method to efficiently engineer crystals, quasicrystals, and liquid crystals by targeting their diffraction patterns. The algorithm combines an evolutionary strategy for parameter optimization with a convolutional neural network as an order parameter, providing a way forward for experimentally feasible colloidal interactions optimized for stabilizing the desired structure.
Article
Chemistry, Physical
Gerardo Campos-Villalobos, Giuliana Giunta, Susana Marin-Aguilar, Marjolein Dijkstra
Summary: This article introduces a method for particle-centered descriptors for non-spherical particle shapes and constructs effective many-body potentials using machine learning techniques. The accuracy of these orientation-dependent many-body potentials is validated through simulations of different model systems.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Susana Marin-Aguilar, Fabrizio Camerin, Marjolein Dijkstra
Summary: The assembly of colloidal cubic diamond is a challenging process. This study explores the conditions for the nucleation of cubic diamond, focusing on the effect of depletion and DNA-mediated interactions. The study finds that a specific balance between the strength and range of depletion interactions enhances the self-assembly of stable cubic diamond.
JOURNAL OF CHEMICAL PHYSICS
(2022)
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)
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
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
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
Physics, Fluids & Plasmas
Carmine Anzivino, Rene van Roij, Marjolein Dijkstra
Summary: Using a grand-canonical Landau-de Gennes theory, this study investigates the local density of twist-bend and splay-bend nematic phases in colloidal suspensions of bent rods. The findings show periodic modulations of local density in the splay-bend phase, making it similar to a smectic phase rather than a nematic phase. In contrast, the twist-bend phase exhibits no spatial variation in local density, confirming it as a proper nematic phase. The predicted density modulations in splay-bend phases are consistent with recent simulations.
