Article
Polymer Science
Daniel L. Vigil, Timothy Quah, Dan Sun, Kris T. Delaney, Glenn H. Fredrickson
Summary: Using self-consistent field theory, the phase boundaries between periodic microphases for linear, comb-like, and bottlebrush diblock copolymers were mapped, revealing a universal phase diagram for sphere phases including A15 and sigma phases. However, a transition from comb-like to bottlebrush scaling with architectural parameter variation was not observed.
Article
Polymer Science
Shifeng Nian, Baiqiang Huang, Guillaume Freychet, Mikhail Zhernenkov, Li-Heng Cai
Summary: Bottlebrush molecules are branched polymers with a densely grafted linear backbone. Contrary to existing understanding, the interbackbone distance in bottlebrush polymers increases as the grafting density of side chains decreases. This discovery provides a paradigm-shifting understanding of the molecular structure of bottlebrush polymers.
Article
Polymer Science
Ignacio Martin-Fabiani, Stavros X. Drakopoulos, Giuseppe Forte, Sylvain Prevost, Ingo Hoffmann, Sara Ronca
Summary: The study using neutron spin echo spectroscopy revealed that graphene oxide hinders chain dynamics in polyethylene melt. The proposed model allows for measurement of adsorbed and free polymer fractions, as well as the thickness of the adsorbed layer. The experiments provided evidence at the nanoscopic level of graphene oxide hindering entanglement formation in the polymer melt.
Article
Polymer Science
So Jung Park, Guo Kang Cheong, Frank S. Bates, Kevin D. Dorfman
Summary: Bottlebrush block copolymers can enhance the stability of the double gyroid phase by increasing segregation strength, while coil-bottlebrush block polymers with architectural asymmetry significantly impact the gyroid stability region. This suggests that architectural asymmetry in bottlebrush block polymers can be a powerful design tool.
Review
Polymer Science
Yumi Matsumiya, Hiroshi Watanabe
Summary: The rheological behavior of polymeric liquids was traditionally believed to be universally determined by a few time-independent molecular parameters, but recent studies have shown non-universality under extensional flow conditions. A key concept is the reduction of segmental friction of highly oriented/stretched polymer chains, which changes with the chemical structure of the polymer and solvent as well as the polymer concentration.
PROGRESS IN POLYMER SCIENCE
(2021)
Article
Mechanics
Martin Zatloukal, Jiri Drabek
Summary: The monomeric friction coefficient for fully aligned chains was determined for three linear isotactic polypropylene melts, showing a significant reduction compared to the equilibrium friction coefficient. This supports the argument that a reduction in the friction coefficient is necessary to understand the dynamics of polymer melts in very fast flows, as suggested by recent rheological data and molecular simulations.
Article
Engineering, Chemical
Sidath Wijesinghe, Dvora Perahia, Ting Ge, K. Michael Salerno, Gary S. Grest
Summary: The stress relaxation of branched polymers, especially the impact of branch length compared to the entanglement length of linear polymer, plays a crucial role in viscosity modification. Shorter branch lengths relax within the entanglement time, affecting chain mobility and stress relaxation by increasing tube diameter and friction coefficient, essentially acting as a solvent in the system.
Article
Polymer Science
Aristotelis Zografos, Helena A. All, Alice B. Chang, Marc A. Hillmyer, Frank S. Bates
Summary: A series of model poly((+/-)-lactide) graft copolymers were synthesized and used to study the transition from star-like to bottlebrush structure in shear and extensional flows. Small-amplitude oscillatory shear and extensional rheometry measurements were conducted on samples with different backbone degrees of polymerization. The transition from star-like to bottlebrush structure occurred at a backbone degree of polymerization between 50 and 69. In extensional flows, the star-like melts exhibited no melt strain hardening, while the bottlebrush melts showed prominent strain hardening. These findings are important for designing bottlebrush materials with strain hardening properties for various processing methods involving extensional flows.
Article
Polymer Science
Katsumi Hagita, Takahiro Murashima, Naoki Sakata, Koya Shimokawa, Tetsuo Deguchi, Erica Uehara, Susumu Fujiwara
Summary: We investigated the topological barriers in ring polyethylene (PE) melts of trefoil knots and found that these barriers prevent crystallization due to self-entanglement. The topological barriers decrease with increasing polymer chain length (N) and the knotted segments are localized in the noncrystallized region. Our study provides insights into the effects of topology on crystallization in polymer melts.
Article
Polymer Science
Heyi Liang, Kenji Yoshimoto, Masahiro Kitabata, Umi Yamamoto, Juan J. de Pablo
Summary: In this study, a multiscale simulation method is used to investigate the rheological properties of entangled Nylon 6 melts. The calculated results agree reasonably with experiments, showing the potential of this approach for designing polymeric materials based on purely molecular models.
JOURNAL OF POLYMER SCIENCE
(2022)
Article
Quantum Science & Technology
Liang Zhang, Chaohan Cui, Jianchang Yan, Yanan Guo, Junxi Wang, Linran Fan
Summary: The researchers have found that the frequency degree of freedom of optical photons can be used for efficient quantum information processing. They have developed an integrated photonic platform for the generation and parallel processing of quantum frequency combs. Through the implementation of cavity-enhanced parametric down-conversion with Sagnac configuration, they were able to generate quantum frequency combs with identical spectral distributions. They also achieved on-chip quantum interference of different frequency modes using the same photonic circuit. This work provides a critical step towards the implementation of efficient quantum information processing with integrated photonics using the frequency degree of freedom.
NPJ QUANTUM INFORMATION
(2023)
Article
Materials Science, Multidisciplinary
Yuji Kinose, Keita Sakakibara, Osamu Sato, Yoshinobu Tsujii
Summary: This article investigated the weak anchoring properties of liquid crystals (LCs) on cross-linked films of PHMA and PEMA bottlebrushes, revealing the mechanism behind the phenomenon. Experimental data and rheological measurements were used to demonstrate the correlation between side chain relaxation dynamics, LC swelling, and phase diagrams of the mixtures. The results showed the interplay between the bottlebrush architecture, cross-linking, and affinity with LCs in explaining the weak anchoring behavior.
ACS APPLIED POLYMER MATERIALS
(2021)
Article
Polymer Science
Karin J. Bichler, Bruno Jakobi, Gerald J. Schneider
Summary: By using dielectric spectroscopy and fast field cycling nuclear magnetic resonance (NMR), the dynamical behavior of different polymer architectures based on PDMS was compared. The segmental dynamics were found to be independent of architecture, but significant differences were observed in large-scale chain dynamics.
Article
Polymer Science
Dong-dong Wang, Xiao-lei Xu
Summary: The stress and structural behaviors of non-entangled comb polymer melts under start-up shear flow were studied and compared with those of linear polymer. The results showed that the stress-strain response of comb polymer is almost the same as that of linear polymer, with only numerical differences. The branch chains of comb polymer have little influence on the rheological behavior.
ACTA POLYMERICA SINICA
(2022)
Article
Quantum Science & Technology
Ming Li, Yan-Lei Zhang, Xin-Biao Xu, Chun-Hua Dong, Guang-Can Guo, Chang-Ling Zou
Summary: This study explores the continuous-variable quantum entanglement of dissipative Kerr soliton combs in microresonators, uncovering two distinct features: entanglement of comb lines at the spectral edge and diminished entanglement at the center of the spectrum.
ADVANCED QUANTUM TECHNOLOGIES
(2023)
Article
Chemistry, Multidisciplinary
Chuao Ma, Jun Wei, Yuqiang Zhang, Xingchao Chen, Chan Liu, Shen Diao, Yuan Gao, Krzysztof Matyjaszewski, Hongliang Liu
Summary: Currently, there is a significant challenge in meeting the increasing demands for conductive ionogels with complex shapes and high processability for next-generation flexible electronics. In this study, highly processable ionogels with mechanical robustness are designed by self-assembly of a common triblock copolymer into a precursor in functional mixed ionic liquids. The viscosity of the self-assembled precursor can be adjusted, making it compatible with various fabrication technologies. By using 3D printing, an auxetic-structured ionogel is easily generated, showing improved sensitivity for monitoring small deformations. This research establishes a new approach for versatile and programmable fabrication of high-performance ionogels, focusing on designing functional mixed ionic liquids rather than synthesizing new polymers.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Engineering, Environmental
Yilin Zhang, Michael R. Martinez, Hui Sun, Mingkang Sun, Rongguan Yin, Jiajun Yan, Benedetto Marelli, Juan Pablo Giraldo, Krzysztof Matyjaszewski, Robert D. Tilton, Gregory V. Lowry
Summary: The understanding of how agrochemical nanocarrier properties affect their uptake and translocation in plants is incomplete. Our study found that anionic nanocarriers were transported at a higher rate than cationic nanocarriers in tomato, while only anionic nanocarriers were transported in wheat. These findings provide design parameters for efficient and targeted agrochemical delivery.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Polymer Science
Andrey V. Dobrynin, Ryan Sayko, Ralph H. Colby
Summary: Viscosity analysis is a valuable technique for polymer characterization. This study proposes a new method to determine the molecular weight of polymers by representing the solution-specific viscosity as a generalized universal function of chain overlap concentration.
Article
Polymer Science
Yuqi Zhao, Rongguan Yin, Hanshu Wu, Zongyu Wang, Yue Zhai, Khidong Kim, Changwoo Do, Krzysztof Matyjaszewski, Michael R. Bockstaller
Summary: Van der Waals-driven self-healing in copolymers with lock-and-key architecture has been achieved by synthesizing lock-and-key copolymers with prescribed sequences. The recovery behavior of copolymers with different sequences was evaluated, and copolymers with alternating and statistical sequences showed a 10-fold increase in recovery rate compared to copolymers with a gradient sequence. The results provide strategies for designing and synthesizing engineering polymers with both structural and thermal stability and the ability to recover from structural damage.
Article
Polymer Science
Kriti Kapil, Shirley Xu, Inseon Lee, Hironobu Murata, Seok-Joon Kwon, Jonathan S. Dordick, Krzysztof Matyjaszewski
Summary: Well-defined multifunctional copolymers with rhodamine B dye were synthesized by ATRP, enabling efficient and specific bioimaging of Staphylococcus aureus. The combination of multifunctional polymeric dyes and strain-specific Ab or CBD showed enhanced fluorescence and target selectivity, making them potential biosensors for the detection of target DNA, protein, or bacteria.
Article
Chemistry, Multidisciplinary
Yilin Zhang, Liye Fu, Michael R. Martinez, Hui Sun, Valeria Nava, Jiajun Yan, Kurt Ristroph, Saadyah E. Averick, Benedetto Marelli, Juan Pablo Giraldo, Krzysztof Matyjaszewski, Robert D. Tilton, Gregory V. Lowry
Summary: Anticipated increases in extreme temperatures can harm crops, but the use of high aspect ratio polymer bottlebrushes can mitigate these effects by delivering stress-regulating agents to plants. These bottlebrushes have shown efficient uptake in leaves and can release encapsulated agents under elevated temperatures, promoting photosynthesis and providing long-term heat stress protection. They can also move through the phloem to protect other plant organs and manage phloem pathogens, making this delivery platform a valuable tool for protecting plants against climate-induced damage.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Jaepil Jeong, So Young An, Xiaolei Hu, Yuqi Zhao, Rongguan Yin, Grzegorz Szczepaniak, Hironobu Murata, Subha R. Das, Krzysztof Matyjaszewski
Summary: This study presents an approach to convert biomass RNA into an acrylic crosslinker by acyl imidazole chemistry, allowing for the fabrication of materials with tunable properties. It also explores reversible-deactivation radical polymerization methods and metallization of the biomass RNA-based material, expanding the opportunities in biomass-based biomaterial fabrication.
Article
Chemistry, Physical
Yuqi Zhao, Hanshu Wu, Rongguan Yin, Chenxi Yu, Krzysztof Matyjaszewski, Michael R. Bockstaller
Summary: The effect of sequence structure on the self-healing and shape-memory properties of copolymer-tethered brush particle films was investigated. It was found that statistical copolymer sequence provided the most rapid restoration of mechanical properties and an increase of the high T(g) (MMA) component improved the material's modulus while retaining self-healing ability. The reduction of flow in brush systems was attributed to slow cooperative relaxation due to the complex microstructure.
CHEMISTRY OF MATERIALS
(2023)
Article
Polymer Science
Krzysztof Jerczynski, Julita Muszynska, Gokhan Demirci, Onur Cetinkaya, Paulina Filipczak, Grzegorz Nowaczyk, Jaroslaw Grobelny, Krzysztof Matyjaszewski, Marcin Kozanecki, Joanna Pietrasik
Summary: This work reports on the efficient performance of hybrid particles with silver nanoparticles distributed within single polymer molecules as Surface Enhanced Raman Scattering (SERS) supports. Through controlled synthesis methods and structure parameters of polymer templates, the researchers successfully synthesized hybrid particles with star-like topology and achieved stable detection of analytes at nanomolar level.
Article
Polymer Science
Andrey V. Dobrynin, Anastasia Stroujkova, Mohammad Vatankhah-Varnosfaderani, Sergei S. Sheiko
Summary: The ability to synthesize elastomeric materials with programmable mechanical properties is crucial for advanced soft matter applications. In this study, a design strategy based on the combination of human intelligence (HI) and artificial intelligence (AI) tools was developed. The strategy allows for precise encoding of mechanical properties by considering three architectural parameters. An artificial neural network (ANN) was trained to predict the mechanical properties of polymer networks based on structure-property cross correlations. The ANN was then used for the synthesis of model networks with identical mechanical properties but different chemistries of network strands.
Article
Polymer Science
Gianluca Gazzola, Irene Filipucci, Andrea Rossa, Krzysztof Matyjaszewski, Francesca Lorandi, Edmondo M. M. Benetti
Summary: Achieving tolerance toward oxygen is essential for the upscalable and technologically relevant processes of fabricating polymer brush-coatings. By judiciously tuning the reaction mixtures and polymerization setup, the compatibility of surface-initiated photoinduced atom transfer radical polymerization (SI-photoATRP) technique can be maximized. Through precise variation of reaction conditions, key parameters like the concentration of Cu-based catalyst and free alkyl halide initiator can be optimized to efficiently consume oxygen and yield uniform and thick brushes, even in more exposed polymerization mixtures.
Article
Materials Science, Multidisciplinary
Ryan Sayko, Michael Jacobs, Marissa Dominijanni, Andrey V. Dobrynin
Summary: By combining the scaling theory of polymer solutions and convolutional neural network (CNN) models, specific parameters were obtained to describe semidilute solution viscosity in different solution regimes. The CNN models were trained on theoretically generated datasets and used to analyze the solution viscosity of various polymers in different solvents. The approach produced accurate results and can be used to predict viscosity based on concentration and polymerization degree.
ACS APPLIED POLYMER MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Mitchell R. Maw, Alexander K. Tanas, Erfan Dashtimoghadam, Evgeniia A. Nikitina, Dimitri A. Ivanov, Andrey V. Dobrynin, Mohammad Vatankhah-Varnosfaderani, Sergei S. Sheiko
Summary: Hot-melt pressure-sensitive adhesives (HMPSAs) are widely used materials in various applications. The traditional formulation of HMPSAs involves the use of thermoplastic elastomers with added plasticizers and tackifiers. However, this study presents an alternative additive-free approach using bottlebrush graft-copolymers that exhibit self-assembly properties and can regulate the adhesive performance through five architectural parameters.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Mitchell Maw, Erfan Dashtimoghadam, Andrew N. Keith, Benjamin J. Morgan, Alexander K. Tanas, Evgeniia Nikitina, Dimitri A. Ivanov, Mohammad Vatankhah-Varnosfaderani, Andrey V. Dobrynin, Sergei S. Sheiko
Summary: In this study, a precise additive-free platform for pressure sensitive adhesive (PSA) design was developed. By utilizing the unique properties of brush-like elastomers, a wide range of adhesion force was achieved with a single polymer chemistry. This approach will be essential for the future implementation of AI technology in molecular engineering of PSAs.
ACS CENTRAL SCIENCE
(2023)