Article
Nanoscience & Nanotechnology
Dong Hyup Kim, Ahram Suh, Geonhyeong Park, Dong Ki Yoon, So Youn Kim
Summary: Nanoscratch-directed self-assembly (DSA) is introduced as a simple and scalable strategy to achieve highly aligned block copolymer (BCP) nanopatterns over a large area, allowing versatile nanofabrication for various functional nanomaterials.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Nanoscience & Nanotechnology
Jiajing Li, Paulina A. Rincon-Delgadillo, Hyo Seon Suh, Geert Mannaert, Paul F. Nealey
Summary: Directed self-assembly of block copolymers has attracted interest from the semiconductor industry due to its potential for achieving semiconductor-relevant structures with a relatively simple and low-cost process. However, the kinetic trapping of self-assembling structures into defective states poses challenges for high-volume manufacturing. A study on the kinetics of defect annihilation in chemoepitaxy DSA revealed a statistical model that suggests all dislocations can be removed by sufficiently long annealing time. Further analysis showed that the distribution of defects is largely influenced by the role of guiding stripes.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Polymer Science
Su Eon Lee, Simon Kim, Jun Hyun Park, Ho Jun Jin, Hwa Soo Kim, Jang Hwan Kim, Hyeong Min Jin, Bong Hoon Kim
Summary: This study demonstrates a novel method to fabricate highly aligned lamellar nanostructures in a millimeter-scale large area by directing the self-assembly of block copolymer (BCP) thin films with a temporary thickness-gradient micropattern via simple two-step thermal annealing. The first step of thermal annealing guides the BCP nanostructure through geometric anchoring, while the second step causes thermal reflow of the height gradient micropattern to flatten it. The shear stress generated by thermal reflow enlarges the grain of the BCP nanostructure, resulting in a highly aligned lamellar pattern over the entire area. Finally, grazing-incidence small-angle x-ray scattering ensures the formation of periodic nanopatterns in large area.
JOURNAL OF POLYMER SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Runze Liu, Hejin Huang, Zehao Sun, Alfredo Alexander-Katz, Caroline A. Ross
Summary: This study presents a method of directed self-assembly using multiple mechanisms to generate well-aligned nanomesh structures, which is then extended to fabricate multi-component metallic structures with 2D/3D hybrid morphologies.
Article
Biochemistry & Molecular Biology
Eunkyung Ji, Cian Cummins, Guillaume Fleury
Summary: This study describes a two-step synthesis method for PLLA-b-PS BBCPs using exo-5-norbornene-2-methanol and exo-5-norbornene-2-carbonyl chloride as initiators, and demonstrates the rapid thin-film self-assembly capabilities of these BBCPs, showing potential for producing different morphologies and nanoporous templates.
Review
Nanoscience & Nanotechnology
Ashish A. Kulkarni, Gregory S. Doerk
Summary: The engineering of light-matter interactions at the nanoscale has revolutionized the design and fabrication of optical materials and devices. Metasurfaces, which are arrays of subwavelength nanostructures that interact with electromagnetic radiation, have become a key platform for ultrathin lenses, displays, polarizers, and other nanophotonic devices. This review highlights the advantages and disadvantages of using block copolymer-based nanopatterning for manufacturing, and discusses recent progress in its application to broadband antireflection, surface enhanced Raman spectroscopy, and other nanophotonic applications. The use of self-assembled block copolymer thin films allows for rapid, inexpensive, and scalable nanophotonic manufacturing on large areas and diverse substrates.
Article
Polymer Science
Yanyan Zhu, Changhang Huang, Liangshun Zhang, David Andelman, Xingkun Man
Summary: The kinetic paths of structural evolution and formation of block copolymer (BCP) particles were investigated using dynamic self-consistent field theory (DSCFT). The study revealed that the self-assembly process of BCP in a poor solvent leads to the formation of striped ellipsoids, onion-like particles, and double-spiral lamellar particles. The shape transition between onion-like particles and striped ellipsoidal ones can be reversible by controlling the temperature and solvent selectivity. Additionally, changing the intermediate bi-continuous structure into a layered one is crucial for the formation of striped ellipsoidal particles.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Polymer Science
Hyeong Min Jin, Su Eon Lee, Simon Kim, Ju Young Kim, Young-Soo Han, Bong Hoon Kim
Summary: This study focuses on using near-infrared laser photothermal treatment to enhance the self-assembly of high-chi block copolymers (BCPs) and achieve highly aligned nanoscale patterned structures on silicon substrates. By controlling the molecular weight and loading metal ions, the formation of highly ordered nanodomains and aligned metal nanowires is successfully achieved. The compatibility of the laser writing process with conventional semiconductor processes is also demonstrated.
JOURNAL OF APPLIED POLYMER SCIENCE
(2022)
Review
Chemistry, Multidisciplinary
Luoxing Xiang, Qian Li, Chen Li, Qiqi Yang, Fugui Xu, Yiyong Mai
Summary: Porous materials with ordered bicontinuous structures have attracted attention due to their ordered periodic structures, efficient mass diffusion, and exceptional optical and magnetic properties. Block copolymer self-assembly is a versatile strategy for preparing these materials.
ADVANCED MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Fei Yu, R. Paxton Thedford, Konrad R. Hedderick, Guillaume Freychet, Mikhail Zhernenkov, Lara A. Estroff, Katja C. Nowack, Sol M. Gruner, Ulrich B. Wiesner
Summary: Recent developments in quantum materials have shown promise in revolutionizing energy and information technologies. By utilizing block copolymers and niobia sol precursors, we successfully prepared mesoporous niobium carbonitride thin film superconductors through a scalable solution processing approach. This cost-effective and scalable method holds great potential for integration into existing microelectronics processing, combining the capabilities of soft matter self-assembly with quantum materials.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Nanoscience & Nanotechnology
Tsung-Lun Lee, Jheng-Wei Lin, Rong-Ming Ho
Summary: This work demonstrates the controlled self-assembly of single-composition block copolymer to fabricate various nanonetwork silica monoliths, with different structures obtained by solvent annealing. Well-ordered nanonetwork SiO2 monoliths were fabricated through templated sol-gel reaction using PS-b-PDMS film as a template.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Nanoscience & Nanotechnology
Jin Yong Shin, Bom Lee, Heo Yeon Lim, Simon Kim, Seong-Jun Jeong
Summary: The proposed TDSA method allows for neutral surface-free vertical orientations of BCP nanopatterns, independent of substrate polarizability, and can generate various morphologies by adjusting trench width and BCP molecular weight. This method has the potential advantage for designing process/device layouts needed for effective manufacturing processes.
Article
Polymer Science
R. Simonutti, D. Bertani, R. Marotta, S. Ferrario, D. Manzone, M. Mauri, M. Gregori, A. Orlando, M. Masserini
Summary: This study investigates the effect of using different common solvents on the self-assembly behavior of block copolymer nanoparticles, finding that the hydrogen bonding ability of the solvent strongly influences the size and shape of the particles, as well as their cytotoxicity.
Article
Polymer Science
Mingyang Chen, Yuguo Chen, Yanyan Zhu, Ying Jiang, David Andelman, Xingkun Man
Summary: We investigated the influence of chain flexibility on the self-assembly behavior of symmetric diblock copolymers (BCPs) in thin film confinement. Using worm-like chain (WLC) self-consistent field theory, we studied the stability of parallel and perpendicular orientations of BCP lamellar phases under varying chain flexibilities. The results showed that the stability of perpendicular lamellae increases with chain rigidity, except for the case of rigid chains on rough substrates where the stability decreases. We also demonstrated the effect of substrate roughness on the critical value of substrate preference for the transition from perpendicular-to-parallel lamellar phases.
Article
Polymer Science
Hanwen Lai, Guangcheng Huang, Xin Tian, Yadong Liu, Shengxiang Ji
Summary: The influence of line width roughness (LWR) and line edge roughness (LER) on the reliability and performance of transistors becomes more and more important in semiconductor fabrication. Directed self-assembly of block copolymers (DSA of BCPs) is a potential solution for next-generation lithography, but more research is needed on the influencing factors of LER and LWR in DSA.
Article
Chemistry, Physical
Marcus Mueller
Summary: Using analytical considerations and particle-based simulations, this study investigates the relaxation of a density modulation in a polymer system without nonbonded interactions. The results demonstrate that shallow density modulations, prepared by different processes but with identical amplitudes and wavevectors, exhibit different nonexponential decay behaviors, challenging the assumption that density alone characterizes the polymer system configuration. Analytic descriptions within Linear-Response Theory (LRT) and the Rouse model are provided, showing quantitative agreement with the particle-based simulations.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Polymer Science
Ishay Columbus, Noga Eren, Renana Elitsur, Maya Davidovich-Pinhas, Roy Shenhar
Summary: This study reports on the preparation of branched supramolecular polymers based on a combination of a bisureidotoluene building block and anionic co-monomers. The results show that branched supramolecular polymers can be obtained by introducing co-monomers with different functionalities. Theoretical analysis suggests that specific interactions convert certain units into branch points, leading to reduced viscosity in the systems. This study expands the methods for controlling the properties of supramolecular polymers and contributes to the development of sophisticated smart materials.
Article
Polymer Science
Cody T. Bezik, Joshua A. Mysona, Ludwig Schneider, Abelardo Ramirez-Hernandez, Marcus Mueller, Juan J. de Pablo
Summary: A new mesophase in binary blends of A-b-(BA')3 miktoarm star block copolymers and A homopolymers has been discovered, consisting of aperiodic discrete domains of A embedded in a continuous matrix of B. Molecular bridging dominates the mechanical behavior of the mesophase, outweighing the influence of microphase segregation. The application of shear leads to a closer structure resembling its speculated discrete nature.
Article
Polymer Science
Noga Eren, Ofer Burg, Elisheva Michman, Inna Popov, Roy Shenhar
Summary: Controlling the complexity in assemblies of metal and semiconductor nanoparticles through the use of asymmetric block copolymer films enables the creation of nanoparticle superstructures with mixed patterns. This opens up new possibilities for the utilization of photonic devices.
Article
Chemistry, Physical
Riham Muzaffar-Kawasma, Meirav Oded, Roy Shenhar
Summary: This study utilizes block copolymer micelles to organize semiconductor nanorods into circularly arranged superstructures. The shape of the micelle templates the arrangement of nanorods and the nanorods exhibit surfactant-like behavior, protecting the micelles from coalescence. The study also explores the influence of micelle attributes on nanorod organization.
Article
Chemistry, Physical
David Steffen, Ludwig Schneider, Marcus Mueller, Joerg Rottler
Summary: This paper investigates the spatiotemporal autocorrelation of shear stress in a supercooled fluid close to the glass transition using molecular dynamics simulations. The results show anisotropic correlations and strongly damped oscillations at non-zero wavevectors. The experimental findings are in good quantitative agreement with a recently developed hydrodynamic theory.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Polymer Science
Gaoyuan Wang, Annette Zippelius, Marcus Mueller
Summary: Cross-linking is a versatile strategy to stabilize the structure and control the dynamics of polymers. This study systematically investigates the phase behavior of randomly cross-linked diblock copolymer melts and reveals the significant influence of the preparation state on the phase diagram.
Article
Polymer Science
Pritam Kumar Jana, Petra Bacova, Ludwig Schneider, Hideki Kobayashi, Kai-Uwe Hollborn, Patrycja Polinska, Craig Burkhart, Vagelis A. Harmandaris, Marcus Mueller
Summary: The theological properties of polymer composites depend on the interfacial interactions between solid fillers and a polymer fluid. This study presents a simulation strategy called the wall-spring thermostat, which uses transient bonds to mimic the interactions between the polymer and the solid surface. The density and lifetime of these transient bonds can be adjusted to control the single-chain and collective dynamics of the polymer at the surface. The simulation technique allows for the capture of dynamic heterogeneities at surfaces.
Article
Chemistry, Physical
Kai-Uwe Hollborn, Ludwig Schneider, Marcus Muller
Summary: Highly coarse-grained (hCG) linear polymer models, based on dissipative particle dynamics (DPD), allow for studying long time and length scales. This top-down strategy uses relevant interactions, such as molecular connectivity, and coarse-grained invariants, like the mean-squared end-to-end distance, to describe the equilibrium behavior of long, flexible macromolecules. However, describing the dynamics of long, entangled polymers is challenging because hCG models do not enforce the noncrossability of molecular backbones. One technique to mimic entanglements in hCG models is slip-springs, which has shown quantitative agreement with simulations, experiments, and theoretical predictions.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Polymer Science
Oliver Dreyer, Gregor Ibbeken, Ludwig Schneider, Niklas Blagojevic, Maryam Radjabian, Volker Abetz, Marcus Mueller
Summary: In this study, the self-assembly of asymmetric diblock copolymers during solvent evaporation was investigated using particle-based Monte Carlo simulations and continuum modeling. The effects of evaporation rate and solvent selectivity on structure formation, particularly the alignment of minority block cylinders, were examined. Comparing the two simulation techniques helped identify general trends with parameter variation and understand the role of single-chain dynamics, fluctuations, and additional model details.
Article
Mathematics, Applied
R. Stenger, S. Herzog, I. Kottlarz, B. Ruechardt, S. Luther, F. Woergoetter, U. Parlitz
Summary: Motivated by cardiac research, this study focuses on reconstructing the dynamics within a spatiotemporal chaotic 3D excitable medium from partial observations at the surface. Three artificial neural network methods are trained to predict deeper layer dynamics from surface observations, using data generated by the Barkley model. The results indicate that cross-prediction is possible, albeit non-trivial, with decreasing quality as prediction depth increases.
Article
Clinical Neurology
Nele Sophie Bruegge, Gesine Marie Sallandt, Ronja Schappert, Frederic Li, Alina Siekmann, Marcin Grzegorzek, Tobias Baeumer, Christian Frings, Christian Beste, Roland Stenger, Veit Roessner, Sebastian Fudickar, Heinz Handels, Alexander Muenchau
Summary: This study aimed to evaluate the performance of modern machine learning approaches in automatically detecting tics in patients with Tourette syndrome based on video recordings. Two different supervised learning methods, manual feature extraction with Random Forest classifier and automated deep neural network, were utilized. The results showed F1 scores of 82.0% (accuracy: 88.4%) for Random Forest and 79.5% (accuracy: 88.5%) for the deep neural network approach. ML algorithms for automatic tic detection based on video recordings are feasible and reliable, and could be valuable for objective tic measurements in clinical trials.
MOVEMENT DISORDERS
(2023)
Article
Chemistry, Physical
Felix Weissenfeld, Lucia Wesenberg, Masaki Nakahata, Marcus Mueller, Motomu Tanaka
Summary: The interactions between vesicle and substrate were investigated using simulation and experiment. Polyacrylic acid brushes with cysteine side chains were grafted onto planar lipid membranes. The addition of Cd2+ ions compacted the polymer brushes and influenced the adhesion of lipid vesicles. Wetting of the vesicles occurred at [CdCl2] = 0.25 mM. The shape and adhesion of vesicles were quantitatively evaluated, and simulations revealed that wetting sensitivity was dependent on the interaction range.
Article
Polymer Science
Niklas Blagojevic, Marcus Mueller
Summary: Using a particle-based model, a free-energy functional, and a lattice model, this study investigates the structure and motion of a grain boundary between two orthogonal grains in asymmetric block copolymers. The study reveals insights into transitions and correlations in space and time. By characterizing the system using a free-energy functional and calculating the minimum free-energy path, the study identifies a minimal set of transitions. The results are used to parametrize a lattice model and investigate grain-boundary motion by kinetic Monte Carlo simulation.
Article
Chemistry, Physical
Meneka Banik, Meirav Oded, Roy Shenhar
Summary: Soft lithography techniques have been widely used to replicate topographic features in polymer films. In this study, these techniques were applied to block copolymer films and resulted in chemical heterogeneity corresponding to the topographic features. Detailed characterization of the patterned films revealed insights into the 3D structure and domain reorganization. The formed structures were successfully utilized for the selective assembly of gold nanoparticles, demonstrating the versatility of this approach in nanofabrication and self-assembly.
