Article
Chemistry, Multidisciplinary
Emma Vargo, Katherine M. Evans, Qingjun Wang, Andrew Sattler, Yiwen Qian, Jie Yao, Ting Xu
Summary: The study demonstrates a straightforward approach to generate ring-shaped nanoparticle assemblies in thin films of supramolecular nanocomposites, simplifying and streamlining nanofabrication processes. Directed self-assembly is used to guide the formation of concentric rings with high-quality orbital angular momentum, introducing interparticle coupling as a new design axis. The detailed analysis confirms the flexibility of the supramolecular system in self-regulating the spatial distribution of components, providing guidelines for developing self-regulating DSA as an alternative to incommensurability-driven methods.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Shuhei Akahori, Takahiro Sasamori, Hiroshi Shinokubo, Yoshihiro Miyake
Summary: The self-assembly behavior of tetraazatetrathia[8]circulenes is revealed to be driven by both enthalpy and entropy, due to the unique structure of the molecules containing sp(2)-hybridized nitrogen atoms.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Physical
Xiaojie Chai, Jianwei Lian, Chao Wang, Xiaobing Hu, Jie Sun, Jun Jiang, Anquan Jiang
Summary: By controlling charge injection, stabilized H-H DWs, NDWs, and T-T DWs were achieved within a LiNbO3 transistor, expanding the application of domain walls in future nano-devices.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Nanoscience & Nanotechnology
Debasree Chowdhury, Shyamal Mondal, Maria Secchi, Maria Caterina Giordano, Lia Vanzetti, Mario Barozzi, Massimo Bersani, Damiano Giubertoni, Francesco Buatier de Mongeot
Summary: Highly porous Ge surfaces with uniformly distributed nanovoid structures were fabricated through ion implantation using a thin silicon nitride layer. By comparing with a flat reference, these nanoporous Ge films demonstrated strong and omnidirectional antireflection properties.
Article
Chemistry, Multidisciplinary
Linna Wang, Shang Shi, Zhang Luo, Na Qu, Bing Liu
Summary: The self-assembly of colloidal rings with tunable asymmetry using a depletion force can create a variety of porous colloidal superstructures, such as microtubes, flexible chains, (plastic) crystals, and highly open liquid crystals. Staged self-assembly in binary or ternary systems leads to the formation of complex ring-in-ring and ring-in-ring-in-ring assemblies, which can further develop into multi-walled microtubes and open columnar liquid crystals. This approach with colloidal rings offers a new pathway for constructing hierarchical and porous ordered metamaterials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Myung-Gyun Baek, Sang-Geon Park
Summary: By introducing self-assembled monolayers, the performance of OLED devices can be improved, and the wetting properties, surface roughness, and work function of the ITO surface can be controlled. SAM-modified devices demonstrate better performance, including higher current density, brightness, and lower turn-on voltage.
Article
Biochemistry & Molecular Biology
Lilian Rodrigues de Oliveira, Douglas de Souza Goncalves, Adriano de Souza Carolino, William Marcondes Facchinatto, Diogo de Carvalho Menezes, Cleverton Oliveira Dias, Luiz Alberto Colnago, Yurimiler Leyet Ruiz, Stefan Talu, Henrique Duarte da Fonseca Filho, Puspitapallab Chaudhuri, Pedro Henrique Campelo, Yvonne Primerano Mascarenhas, Edgar Aparecido Sanches
Summary: A systematic investigation of the crystallization process of Poly(p-anisidine) (PPA), a polyaniline derivative, was conducted using experimental and theoretical methods. The results revealed different degrees of crystallinity and crystal structures, with needle and globular morphologies observed. Multifractal analysis showed increased complexity of the PPA surface as the crystallinity decreased. High-resolution C-13 NMR results supported the proposed molecular structures of PPA.
Article
Materials Science, Multidisciplinary
Bin Mu, Jian Chen, Keyang Chen, Chunxiu Zhang, Dongzhong Chen
Summary: This study successfully designed liquid-crystalline dendrimers with donor triphenylene as the peripheral discotic mesogen and acceptor fullerene as the dendrimer core, achieving heterojunction ambipolar charge-transport columnar materials. The resulting donor-acceptor segregated columnar materials exhibit ambipolar charge-transport behavior with high mobilities for both holes and electrons.
JOURNAL OF MATERIALS CHEMISTRY C
(2021)
Article
Chemistry, Multidisciplinary
Li-Hua Yu, Zhen-Feng Cai, Lander Verstraete, Yuanzhi Xia, Yuan Fang, Louis Cuccia, Oleksandr Ivasenko, Steven De Feyter
Summary: This study investigates the impact of covalent modification on the self-assembly of a quinonoid zwitterion derivative. It is found that covalent modification can induce the formation of self-assembled structures at low concentrations, where no self-assembly behavior is observed on the bare surface. The size of the self-assembled domains decreases with increasing the density of grafted molecules, and the dynamics of domains, including growth, shrinkage, and orientation conversion, are captured with molecular resolution.
Article
Polymer Science
Noora Al Balushi, Mitchell Boyd-Moss, Rasika M. Samarasinghe, Aaqil Rifai, Stephanie J. Franks, Kate Firipis, Benjamin M. Long, Ian A. Darby, David R. Nisbet, Dodie Pouniotis, Richard J. Williams
Summary: Metastatic tumors are complex ecosystems consisting of multiple cell types that exist within a specific microenvironment. The interactions between these cells and the signals in the microenvironment play a crucial role in determining tumor behavior. A novel functional model has been developed to mimic the biological, chemical, and contextual cues of a tumor in vivo, allowing for a better understanding of tumor progression and spread within the microenvironment.
Article
Physics, Multidisciplinary
Emanuele Locatelli, Valentino Bianco, Paolo Malgaretti
Summary: Through numerical simulations, it has been found that the conformations of isolated active ring polymers exhibit size-dependent behavior, with short rings swelling and longer rings collapsing under high activity. The study identifies a universal route driving both outcomes and emphasizes the central role of steric interactions and topology conservation. Additionally, it is observed that the collapsed rings are arrested, indicating the presence of extremely long timescales at the steady state, associated with the internal dynamics of the collapsed section.
PHYSICAL REVIEW LETTERS
(2021)
Article
Multidisciplinary Sciences
Thomas Litschel, Charlotte F. Kelley, Danielle Holz, Maral Adeli Koudehi, Sven Kenjiro Vogel, Laura Burbaum, Naoko Mizuno, Dimitrios Vavylonis, Petra Schwille
Summary: Researchers have successfully studied bundled actin filaments in Giant Unilamellar Vesicles using advanced encapsulation methods and compared the results with theoretical modeling. By changing key parameters, they were able to simulate actin polymerization to resemble various types of networks in living cells.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Herbert Levine, Daniel I. Goldman
Summary: We propose the integration of active matter physics with principles of regulatory interactions and control to develop a field called smart active matter. This field can provide insights into important principles in living systems and aid in the engineering of responsive, robust, and functional collectives.
Article
Biochemistry & Molecular Biology
Daniel Major, Lara Flanzbaum, Leah Lussier, Carly Davies, Kristian Mark P. Caldo, Jeella Z. Acedo
Summary: Genome mining and gene cluster analysis were used to identify novel head-to-tail cyclized bacteriocins, revealing a greater diversity than previously thought. The approach proved more effective than traditional bioprospecting, laying the groundwork for future isolation of new head-to-tail cyclized bacteriocins.
Article
Chemistry, Physical
Santiago Gomez Melo, Dennis Woerthmueller, Pierre Gonczy, Niccolo Banterle, Ulrich S. Schwarz
Summary: SAS-6 self-assembles into rings on a surface, ensuring the nine-fold symmetry of centriole organelle. Simulation and experimental comparison show that weak interaction energies and small angular range are necessary for the selection of nine-fold symmetry.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Nanoscience & Nanotechnology
Zongzhe Li, Miguel A. Soto, James G. Drummond, D. Mark Martinez, Wadood Y. Hamad, Mark J. MacLachlan
Summary: This study reports a novel strategy to synthesize cellulose nanocrystal (CNC) gels with tunable mechanical properties. By applying sequential freeze-thaw cycling and hydrothermal treatments, a series of pristine CNC hydrogels and lightweight CNC aerogels were successfully prepared. The mechanical, microstructural, and thermal properties of these materials were investigated, demonstrating their potential applications in various fields.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Miguel A. Soto, Veronica Carta, Ingrid Suzana, Brian O. Patrick, Francesco Lelj, Mark J. MacLachlan
Summary: Macrocycle engineering is a key topic in supramolecular chemistry. This study combines different approaches and post-synthetic modifications to transform a single tether into multiple rings. The macrocycles undergo redox reactions, allowing for control of conformational changes and host activity, enabling the capture and release of guests, ring transformations, and control of pseudorotaxane-to-pseudorotaxane conversions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemistry & Molecular Biology
Lucas J. Andrew, Christopher M. Walters, Wadood Y. Hamad, Mark J. MacLachlan
Summary: Composite films of cellulose nanocrystals (CNCs) and polymers were prepared by solvent evaporation, and the effects of different polymers on CNC self assembly were investigated. It was found that PVP physically adsorbs to the surface of CNCs, resulting in a blue shift in film color with increasing concentration and polymer molecular weight. PEG induces depletion interactions that decrease the size of chiral nematic CNC domains, but has negligible effect on film color. PAA hydrogen bonds to the hydroxyl groups of CNCs, resulting in a blue shift in color along with interesting rheological and liquid-state properties.
Article
Engineering, Biomedical
Andreia Leal Pereira, Angela Semitela, Andre F. Girao, Antonio Completo, Paula A. A. P. Marques, Samuel Guieu, Maria Helena V. Fernandes
Summary: One tissue engineering strategy involves creating scaffolds that resemble the extracellular matrix (ECM) to aid tissue regeneration. In this study, a technique called thermally-induced self-agglomeration (TISA) was used to convert two-dimensional electrospun membranes into highly functional three-dimensional porous-fibrous systems, overcoming the limitations of cell infiltration and proliferation. By electrospinning polycaprolactone/chitosan blends and adjusting the amount of chitosan, the researchers were able to modulate the properties of the resulting 3D nanofibrous scaffolds, leading to porous constructs with distinct morphologic and mechanical features. Viability and proliferation studies with adult human chondrocytes confirmed the biocompatibility of the scaffolds, making them promising for musculoskeletal tissue engineering applications, particularly cartilage repair.
JOURNAL OF BIOMEDICAL MATERIALS RESEARCH PART A
(2023)
Review
Biochemistry & Molecular Biology
Joana R. M. Ferreira, Catia I. C. Esteves, Maria Manuel B. Marques, Samuel Guieu
Summary: The Green Fluorescent Protein (GFP) and its analogues are widely used as fluorescent biomarkers in cell biology. However, the fluorescence of the GFP chromophore is not emitted when it is isolated in solution outside the protein environment. This review discusses various strategies that have been developed to hinder torsional rotations and achieve highly emissive GFP chromophore.
Article
Chemistry, Organic
Joana R. M. Ferreira, Mariana Alves, Barbara Sousa, Sandra I. Vieira, Artur M. S. Silva, Samuel Guieu, Angela Cunha, Raquel Nunes da Silva
Summary: Fluorescence imaging is widely used to study living organisms, but it is challenging to visualize fungi using this method due to their cell wall acting as a diffusion barrier and limited availability of synthetic organic dyes. To address this, a family of curcumin-based boron diketonate complexes was synthesized, allowing for visualization of fungi in different colors without noticeable toxicity. These probes readily entered cells and precisely localized in sub-cellular organelles.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Mingcong Xu, Zhen Xu, Miguel A. Soto, Yi-Tao Xu, Wadood Y. Hamad, Mark J. MacLachlan
Summary: This study demonstrates that cellulose nanocrystal shape-memory polymers (CNC-SMPs) with luminescent components enable mechanically responsive circularly polarized luminescence (CPL). The chiral nematic organization of CNCs in the material allows for precise control of CPL emission with varied wavelengths and high dissymmetry factors (g(lum)). Moreover, colorimetric and CPL-active patterns are created by imprinting desired forms into SMP samples. This study presents a novel way to fabricate smart CPL systems using biomaterials.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Miguel A. Soto, Mohammad T. Chaudhry, Gunwant K. Matharu, Francesco Lelj, Mark J. MacLachlan
Summary: Despite their unique potential, metal-metal bonds have seldom been studied as active components in supramolecular assemblies. In this research, a dynamic molecular container named "flytrap" was constructed using Pt-Pt bonds, and its flexible jaw can adapt to bind large inorganic cations. The flytrap was characterized spectroscopically and crystallographically, and its photochemical assembly was reported, which enables the capture and transport of ions. Additionally, the reversible nature of the Pt-Pt bond allows for the regeneration of the flytrap's starting material. The advances presented here could be applied to assemble other molecular containers and materials for substrate harvesting from solution.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Kyoungil Cho, Lucas J. Andrew, Mark J. MacLachlan
Summary: Zeolitic imidazolate framework (ZIF-8) nanocrystals were grown uniformly on cellulose nanocrystals (CNCs) surface to produce ZIF@CNCs hybrid material. By adjusting the component stoichiometry, the size of ZIF-8 crystals on CNC surface could be controlled. ZIF@CNC-2 was optimized and used as a template to synthesize microporous organic polymer (MOP), ZIF@MOP@CNC. After etching ZIF-8, a MOP material with enclosed CNCs (MOP@CNC) was formed. Zinc coordination into MOP porphyrin unit resulted in ship-in-a-bottle structure, Zn MOP@CNC, where CNCs were encapsulated within Zn-MOP. Compared to ZIF@CNC-2, Zn MOP@CNC exhibited superior catalytic activity and chemical stability for CO2 fixation, converting epichlorohydrin to chloroethylene carbonate. This work presents a novel method of creating porous materials using CNC templating.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Francesco D'Acierno, Carl A. Michal, Mark J. MacLachlan
Summary: This article provides a comprehensive literature review on the thermal stability of cellulose nanomaterials (CNMs). It identifies five major factors affecting CNMs' thermal stability and establishes a quantitative relationship between thermal stability and seven variables using multiple linear least-squares regression. The findings of this study can guide the design of CNMs with predictable thermal properties and the identification of optimal conditions for achieving high thermal stability.
Article
Chemistry, Multidisciplinary
Lucas J. Andrew, Emma R. Gillman, Christopher M. Walters, Erlantz Lizundia, Mark J. MacLachlan
Summary: This paper presents a novel chiral nematic activated carbon aerogel material based on renewable cellulose, which exhibits high specific surface area and superparamagnetic behavior, making it suitable for supercapacitor applications.
Article
Nanoscience & Nanotechnology
Madhureeta Das Gupta, Charlotte E. Boott, Jennifer E. Goon, Brian O. Patrick, Mark J. MacLachlan, Jolene P. Reid
Summary: Supramolecular nanofibers with a narrow length distribution were obtained through the self-assembly of a tris-salphen complex. The length of the nanofibers could be easily adjusted while maintaining low dispersity by controlling the self-assembly conditions. Crystal structure analysis and density functional theory calculations indicated the presence of a metastable aggregate, which transforms into longer supramolecular nanofibers upon heating. The controlled molecular assembly of these complexes may have significant implications for catalysis, electronics, and optical applications.
ACS APPLIED NANO MATERIALS
(2023)
Review
Chemistry, Multidisciplinary
Luis F. B. Fontes, Joao Rocha, Artur M. S. Silva, Samuel Guieu
Summary: The effective utilization of luminescent dyes requires a comprehensive understanding of their excitation and relaxation pathways, including Excited-State Proton Transfer (ESPT). Experimental demonstration of ESPT can be challenging due to competing phenomena. A holistic approach, integrating experimental results, computational analysis, and diverse mechanism assessment, is crucial for verifying the occurrence of ESPT.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Zongzhe Li, Karl Tsang, Yi-Tao Xu, James G. G. Drummond, D. Mark Martinez, Mark J. J. MacLachlan
Summary: Understanding the fundamental properties of chiral nematic cellulose nanocrystal (CNC) aerogels is crucial for expanding their potential applications. We report on the directional thermal and mechanical properties of CNC aerogels and have discovered unexpected differences in thermal conductivity and mechanical strength between different surfaces. These findings are important for understanding the nature of CNC aerogels and expanding their potential applications.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Inorganic & Nuclear
Huan Gao, Miguel A. Soto, Joanna K. Szymkowiak, Lucas J. Andrew, Wadood Y. Hamad, Mark J. MacLachlan
Summary: In this study, halloysite nanotubes (HNTs) were incorporated into cellulose nanocrystal (CNC) films to prepare organic-inorganic composite films with enhanced mechanical properties and maintained iridescence. The hybrid composite films containing 10 wt% HNTs exhibited increased elasticity, with a 1.3-fold increase in tensile strength and a 1.6-fold increase in maximum strain compared to pristine CNC films. Additionally, the incorporation of HNTs slightly improved the thermal stability of the composite films. These materials mimic the hybrid composite structures of crab shells and provide enhanced mechanical properties and thermal stability for CNC films while preserving iridescence.
DALTON TRANSACTIONS
(2023)