Article
Chemistry, Multidisciplinary
Lorenza Spina, Federica Ciuchi, Caterina Maria Tone, Riccardo Barberi, Maria Penelope De Santo
Summary: This study investigates chirality in chromonic liquid crystals by doping with a strong helical-twisting-power peptide and confining in a spherical geometry. The results show that the geometrical constraint and the presence of the chiral dopant enhance the chiral effect, leading to a highly ordered helical superstructure. Additionally, the study demonstrates the potential for creating biocompatible and eco-friendly optical devices for sensor and anticounterfeiting applications.
Article
Multidisciplinary Sciences
Jie Liu, Wenzhe Liu, Bo Guan, Bo Wang, Lei Shi, Feng Jin, Zhigang Zheng, Jingxia Wang, Tomiki Ikeda, Lei Jiang
Summary: By intercepting nucleation processes with fast cross-linking of a stabilizing polymer matrix, the transformation of cholesteric liquid crystal blue phases was achieved. The study revealed highly coordinated, diffusionless transformations of the grid of double-twisted cylinders, providing promising templates for photonic crystals and discussing potential applications.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
James Jennings, Georg Pabst
Summary: In this article, a high-throughput synthesis of lipidoids that assemble into liquid crystalline phases is conducted. The screening approach leads to the discovery of 12 different lipidoid structures capable of forming bicontinuous double gyroid phases. Unexpected design criteria for phase selection are uncovered through small-angle X-ray scattering (SAXS) data. Two examples of functional materials from lipidoid liquid crystals are demonstrated.
Article
Chemistry, Multidisciplinary
Tadej Emersic, Kushal Bagchi, Jose A. Martinez-Gonzalez, Xiao Li, Juan J. de Pablo, Paul F. Nealey
Summary: It is experimentally demonstrated that chemical patterns can direct the self-assembly of blue phases (BPs), regardless of the chemistry and complexity of the material. This suggests that a thermodynamics-based continuum description can be applied to a broad range of materials for the self-assembly of BPs.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Physical
P. Romero-Hasler, E. A. Soto-Bustamante
Summary: A series of acrylic phenyl benzoate polymers with high molecular weight were synthesized and characterized using a novel polymerization method. Characterization methods included polarized optical microscopy, differential scanning calorimetry, and wide-angle X-ray scattering. All polymers exhibited liquid crystal phases, with some showing nematic phases and others showing smectic phases depending on the chain length. The transition from monolayer to bilayer smectic phase was observed when polymerizing a monomer with a terminal chain length of five carbon atoms.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Review
Chemistry, Multidisciplinary
Nadia Kapernaum, Alyna Lange, Max Ebert, Marco A. Grunwald, Christian Haege, Sebastian Marino, Anna Zens, Andreas Taubert, Frank Giesselmann, Sabine Laschat
Summary: Ionic liquid crystals (ILCs) have attracted significant attention due to their mesomorphic, liquid crystalline, and anisotropic properties. Recent research focuses on fundamental aspects, synthesis variations, and tuning of mesomorphic behavior of ILCs. Challenges ahead include commercialization and overcoming technical obstacles in the field.
Article
Chemistry, Multidisciplinary
Niamh Mac Fhionnlaoich, Stephen Schrettl, Nicholas B. Tito, Ye Yang, Malavika Nair, Luis A. Serrano, Kellen Harkness, Paulo Jacob Silva, Holger Frauenrath, Francesca Serra, W. Craig Carter, Francesco Stellacci, Stefan Guldin
Summary: In this study, the collective self-assembly of gold nanoparticles in a thermotropic liquid crystal driven by a temperature-induced phase transition was reported. The transition from the isotropic to the nematic phase resulted in the assembly of nanometer-sized particles into arrays of micrometer-sized agglomerates, with the size and spacing controlled by the cooling rate. Phase field simulations showed similar morphology evolution as the experimental observations. This reversible process offers control over structural order on the microscopic level and has potential applications in programmable and reconfigurable nanocomposites with micrometer-sized periodicities.
Article
Chemistry, Multidisciplinary
Zhen Shan, Miaomiao Wu, Dongyang Zhu, Xiaowei Wu, Kan Zhang, Rafael Verduzco, Gen Zhang
Summary: This study presents the successful design and synthesis of an aporphyrin-based 8-connected building block, greatly enriching the topological possibilities of 3D COFs.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Sergei Vereshchagin, Vyacheslav Dudnikov, Yury Orlov, Leonid Solovyov
Summary: Processes of ordering and disordering of Sr2+/Dy(3+) cations in a single-phase Sr0.8Dy0.2CoO3-delta were investigated using TG-DSC and XRD techniques. The characteristics of the ordered-disordered phase transition were found to be highly sensitive to the cooling rate.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Chemistry, Physical
Supreet Kaur, Nazma Begum, Golam Mohiuddin, Santanu Kumar Pal
Summary: The study presented here investigates the photoswitching behavior of azobenzene-based polar hockey-stick-shaped liquid crystals (HSLCs) by synthesizing two new series of phenyl-ring based polar HSLCs. The synthesized materials exhibited decent photochromic behavior and different potential applications. The thermal phase behavior of the superstructural assembly was characterized using various techniques, revealing the formation of nematic and partially bilayer smectic A phases depending on the length of the terminal alkyl chain.
Article
Chemistry, Physical
Pezhman Mohammadi, Fabian Zemke, Wolfgang Wagermaier, Markus B. Linder
Summary: This study investigates the self-assembly process of recombinant proteins inspired by spider silk, showing the formation of an elastic skin at the water-air interface with high concentration of beta-sheets over time. The beta-sheet formation strongly depends on protein concentration and relative humidity, influencing both the amount and ordering of these structures during the process.
Article
Chemistry, Multidisciplinary
Katarina Gvozden, Sanja Novak Ratajczak, Alberto G. Orellana, Emmanuel Kentzinger, Ulrich Rucker, Jan K. G. Dhont, Cristiano De Michele, Emmanuel Stiakakis
Summary: Stiff DNA fragments can self-assemble into various smectic mesophases in concentrated aqueous solutions by selectively screening blunt-end DNA stacking interactions. The strength of attractions can be controlled to stabilize different phases, demonstrating the potential for precise tuning of DNA blunt-ends as monovalent attractive patches in the assembly of nonconventional DNA-based liquid crystal phases.
Article
Chemistry, Applied
Xue Xia, Cai-Li Zhao, Hong-Tian Xu, Wen-Hao Yu, Shi-Kai Xiang, Lai-Cai Li, Ke-Qing Zhao, Chun Feng, Bi-Qin Wang
Summary: This article describes the synthesis and self-assembly behavior of a series of ten optically active triphenylenedicarboxyimide (TDI) derivatives with a stereogenic center. The TDIs show an enantiotropic hexagonal columnar mesophase with high clearing temperatures. Chiral supramolecular structures are observed in the columnar mesophase of three pairs of chiral TDIs. The axially connected aromatic ring at the stereocenter provides steric repulsion upon stacking, leading to the formation of chiral supramolecular structures. The configuration of the stereogenic center is not the only factor responsible for inducing helical structures in solution.
Article
Physics, Multidisciplinary
Paul Loubeyre, Florent Occelli, Paul Dumas
Summary: This study investigates the influence of nuclear quantum fluctuations on the properties of dense hydrogen, focusing on its potential metallization. Raman spectroscopy and synchrotron infrared absorption measurements are conducted on deuterium at 460 GPa and 80 K, revealing the isotopic effects on the electronic and vibrational properties in phase III. The findings also suggest a probable transition to metal deuterium, occurring at a shifted pressure compared to hydrogen, and are compared to advanced calculations quantifying the reduction of the band gap caused by nuclear quantum fluctuations.
PHYSICAL REVIEW LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Sepideh Norouzi, Antonio Tavera-Vazquez, Johanan Ramirez-de Arellano, Dae Seok Kim, Teresa Lopez-Leon, Juan J. de Pablo, Jose A. Martinez-Gonzalez, Monirosadat Sadati
Summary: This study investigates the crystallization behavior of blue phase liquid crystals under curved confinement. The results show that the high curvature and spatial confinement can lead to the reconfiguration of the BPI phase into the BPII phase, resulting in different optical characteristics and structural morphologies. Additionally, the coupling of curvature and confinement leads to the nucleation of skyrmions at greater thicknesses.
Article
Chemistry, Multidisciplinary
Yang-yang Zhao, Yaxin Li, Yu Cao, Georg H. Mehl, Feng Liu, Goran Ungar
Summary: The correlation between the size of nanoparticles, the structure and shape of mesogenic ligands and the ensuing assembly behaviour is not fully understood. In this study, gold nanoparticles of different sizes were synthesized and modified with ligands containing rod-like mesogens. The resulting structures were compared and analyzed, and general rules were derived to assist in designing the soft corona of nanoparticles to achieve desired structures and anisotropy.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Kazuma Hamaguchi, Huanjun Lu, Shota Okamura, Satoshi Kajiyama, Junya Uchida, Shunsuke Sato, Go Watanabe, Yoshiki Ishii, Hitoshi Washizu, Goran Ungar, Takashi Kato
Summary: In this study, a combined experimental and computational approach was used to investigate the self-assembly and reentrant behavior of a single-component thermotropic liquid crystal for dynamically functional materials. A designed mesogenic molecule with an unprecedented sequence of layered smectic phases was synthesized, and it exhibited switching functions due to competition between mesogen stacking and conformational flexibility. Ion-conductive reentrant liquid-crystalline materials, showing multistep conductivity changes, were developed.
Article
Polymer Science
Haohui Huo, Jing Zou, Shu-Gui Yang, Jiaqi Zhang, Jie Liu, Yutong Liu, Yanyun Hao, Hongfei Chen, Hui Li, Chaobo Huang, Goran Ungar, Feng Liu, Zhiyue Zhang, Qilu Zhang
Summary: In this study, novel multicompartment nanoparticles (MCNs) with high stability and cargo loading capacity were developed using crystallization-driven self-assembly (CDSA) method. The MCNs exhibited excellent encapsulation capability for hydrophobic drugs and demonstrated cytocompatibility and dose-dependent cellular uptake and cytotoxicity.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Polymer Science
Jiaining Cui, Qilu Zhang, Feng Liu, Shu-Gui Yang, Goran Ungar
Summary: The formation of stereocomplex crystals (SC) is an effective method to enhance the heat resistance and mechanical performance of poly(lactic acid) products. However, the SC crystallization of a high-molecular-weight poly(L-lactic acid)/poly(D-lactic acid) (PLLA/PDLA) racemate stops or does not start at high temperatures, leading to the crystallization of homochiral crystals (HC) or an SC-HC mixture on cooling. This phenomenon is caused by the accumulation of the pure enantiomer that is rejected from the SC growth front, which is a result of random compositional fluctuation in the melt. The growth of SC can be resumed at lower temperatures along with the growth of HC, and the problem is mainly in growth rather than nucleation.
Article
Polymer Science
Shu-Gui Yang, Liang-Qing Zhang, Jiaming Cui, Xiang-bing Zeng, Baolin Guo, Feng Liu, Goran Ungar
Summary: This study used two-photon confocal laser microscopy to obtain three-dimensional images of the morphology of poly(lactic acid) after shear-induced crystallization. By doping the polymer with Nile Red, the necessary fluorescence contrast was achieved. The results showed that the shape of the resulting cylindrites, or large-diameter shish-kebabs, was influenced by the shear method used. Additionally, the formation of a row of spherulites was observed during fiber pull, which was attributed to crystallization-induced volume contraction.
Article
Polymer Science
Yanlin Shi, Sung-Po R. Chen, George Fragkiadakis, Daniele Parisi, Virgil Percec, Dimitris Vlassopoulos, Michael J. Monteiro
Summary: The shape, breadth, and average molecular weight of the overall molecular weight distribution (MWD) are important for determining polymer properties. Traditional methods can only achieve desired Gaussian distribution through complex modeling, while living radical polymerization provides a simpler route. Blending low-reactive RAFT agents allows the construction of square, slanted, and chair-like MWDs, providing control over MWD shape and breadth. This blending method overcomes difficulties in producing unusual MWDs and offers a general synthetic strategy for studying structure-property relationships of polymers.
Article
Polymer Science
Virgil Percec, Dipankar Sahoo, Jasper Adamson
Summary: This article organized for the first time the stimuli-responsive principles of supramolecular organizations emerging from self-assembling and self-organizable dendrons, dendrimers, and dendronized polymers, which is fundamental to natural and life sciences.
Article
Polymer Science
Adrian Moreno, Gerard Lligadas, Jasper Adamson, Devendra S. Maurya, Virgil Percec
Summary: The Nobel Prize in Chemistry for 2022 was awarded to Bertozzi, Meldal, and Sharpless for their contribution to the development of click chemistry and biorthogonal chemistry. Since 2001, when click chemistry was proposed by Sharpless's laboratory, synthetic chemists have favored click reactions as a preferred method to create new functions. This perspective summarizes the research conducted in our laboratories on CuAAC, TBC, and TERMINI click reactions, and their applications in assembling complex macromolecules and self-organizations with biological relevance.
Article
Pharmacology & Pharmacy
Juncheng Lu, Elena N. Atochina-Vasserman, Devendra S. Maurya, Muhammad Irhash Shalihin, Dapeng Zhang, Srijay S. Chenna, Jasper Adamson, Matthew Liu, Habib Ur Rehman Shah, Honey Shah, Qi Xiao, Bryn Queeley, Nathan A. Ona, Erin K. Reagan, Houping Ni, Dipankar Sahoo, Mihai Peterca, Drew Weissman, Virgil Percec
Summary: The use of viral and synthetic vectors for nucleic acid delivery is crucial for the rapid development of effective COVID-19 vaccines. Lipid nanoparticles (LNPs) composed of phospholipids, PEG-conjugated lipids, cholesterol, and ionizable lipids have been employed as the leading nonviral delivery vector for COVID-19 mRNA vaccines by BioNTech/Pfizer and Moderna. In this study, a methodology involving screening libraries was used to discover the molecular design principles necessary for targeted mRNA delivery to specific organs, using a one-component ionizable multifunctional amphiphilic Janus dendrimer (IAJD) derived from plant phenolic acids. These design principles simplify the synthesis of IAJDs and the assembly of monodisperse dendrimersome nanoparticles (DNPs) with predictable dimensions, ultimately enhancing accessibility to diverse mRNA-based vaccines and nanotherapeutics.
Article
Chemistry, Multidisciplinary
Dipankar Sahoo, Emad Aqad, Mihai Peterca, Virgil Percec
Summary: This publication reports the structural analysis of the 3D self-organizations of HATn molecules, revealing the formation of highly ordered helical and nonhelical pyramidal and discotic columns. It demonstrates that a single building block can self-organize into different assemblies via its constitutional isomers. The findings raise important questions about the current understanding of helical self-organizations.
Article
Chemistry, Multidisciplinary
Dipankar Sahoo, Emad Aqad, Mihai Peterca, Virgil Percec
Summary: The molecular structures of 3D crystal and 2D liquid crystal phases of discotic molecules have never been determined at the molecular level. This study investigates the molecular structure of HATn self-organizations and presents the molecular structures of HAT4 in its crystal and liquid crystal states.
Article
Chemistry, Multidisciplinary
Ningdong Huang, Weiheng Huang, Zhenlin Luo, Wangsheng Chu, Goran Ungar
Summary: 3D crystalline order with 1 nm resolution is observed in aqueous solutions of supramolecular nanotubes containing 94% water, at concentrations as low as 6 wt%. The nanotubes are formed by supramolecular rings of star-like organic ions, which stack on top of each other to form long hollow tubes with 15 nm outer diameter. The high 3D order is attributed to long-range attraction between like-charged tubes and amplified charge modulation by the extremely high intra-tube correlation length.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)