Review
Materials Science, Multidisciplinary
Xue Li, Chen Chen, Qian Niu, Nian-Wu Li, Le Yu, Bao Wang
Summary: This review summarizes the self-assembly of nanoparticles at solid-liquid interface, including different driving forces, types of assembly, and applications in electrochemical capacitors.
Article
Chemistry, Multidisciplinary
Hongjie Xu, Yujie Su, Chenggong Zheng, Yuchen Wang, Yuping Tong, Zhongzheng Yang, Junhua Hu
Summary: This review discusses the interplay between theoretical calculation and experiment in the study of lithium ion battery materials. The application of theoretical calculation method in solid-state batteries is introduced, and the concept and assembly technology of solid-state batteries are reviewed. The analysis of basic parameters of solid-state electrolytes, especially sulfide-based solid-state electrolytes and their interface mechanisms with high-voltage cathode materials, is carried out using theoretical methods. The review also presents an overview on the scientific challenges, fundamental mechanisms, and design strategies for solid-state batteries, with a focus on stability issues of solid-state electrolytes and associated interfaces.
CHINESE CHEMICAL LETTERS
(2024)
Article
Chemistry, Inorganic & Nuclear
Pavel A. Tarakanov, Anton O. Simakov, Victor E. Pushkarev, Dmitry V. Konev, Olga A. Goncharova, Nikita A. Slesarenko, Ekaterina N. Tarakanova, Sergey E. Nefedov, Pavel A. Stuzhin
Summary: A series of 5,7-disubstituted 1,4-diazepinoporphyrazinato magnesium(ii) and nickel(ii) complexes, including two novel compounds, were obtained by metal-templated macrocyclization. Their tendency towards H-type dimerization was studied using various techniques, and the influence of structural and solvation factors on dimer stability was traced.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Physical
Lander Verstraete, Tamara Rinkovec, Hai Cao, Hywel Reeves, Jeremy N. Harvey, Steven De Feyter
Summary: The study reveals that when the length of n-alkane chains reaches a certain value, the lattice mismatch between them and graphite will induce a conformational change from the classical straight chain to a twisted, chiral chain. This crossover is experimentally and computationally determined to occur between 40 and 50 carbon atoms.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Nanoscience & Nanotechnology
Liwen Zhang, Malgorzata Kowalik, Qian Mao, Behzad Damirchi, Yongyi Zhang, Philip D. Bradford, Qingwen Li, Adri C. T. van Duin, Yuntian T. T. Zhu
Summary: Stress graphitization is observed at the carbon nanotube (CNT)-matrix interfaces in CNT/carbon matrix (CNT/C) composites. However, the lack of understanding about its evolution mechanisms and the gap between theory and experiment have hindered the development of high-performance CNT/C composites. In this study, molecular dynamics simulations and experiments were conducted to investigate the stress graphitization mechanisms in a CNT/polyacrylonitrile (PAN)-based carbon matrix composite. The results provide atomistic insights into stress graphitization and offer guidance for optimizing CNT-matrix interfaces to develop novel CNT/C composites with improved performance.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Yuan Fang, Oleksandr Ivasenko, Ana Sanz-Matias, Kunal S. Mali, Kazukuni Tahara, Yoshito Tobe, Steven De Feyter
Summary: Self-assembled molecular networks (SAMNs) are spontaneously formed through the assembly of molecules on surfaces. Scanning tunneling microscopy (STM) can track their growth dynamics on conductive atomically flat surfaces and at the liquid-solid interface. Desorption and adsorption dynamics are challenging to investigate through the liquid-solid interface. Porous molecular networks have attracted particular interest as they can act as platforms for sensing and host-guest chemistry. However, their stability in a liquid environment is still poorly understood. In this study, the authors investigated the desorption/adsorption dynamics of supramolecular porous monolayers at the interface between highly oriented pyrolytic graphite and 1-phenyloctane, and revealed the time scales, temperature dependence, and the role of STM tip in inducing dynamics.
Article
Chemistry, Multidisciplinary
Govind P. Maurya, Deepak Verma, Aloka Sinha, Luc Brunsveld, V Haridas
Summary: This study demonstrates the synthesis of simple and tunable hydrophobically driven chiral functional assemblies of diacetylene cored pseudopeptides. The chiral appended amino acid elements and the hydrophobic dialkyne core play important roles in the self-assembly and aggregation induced emission properties of these materials. Moreover, these supramolecular materials show promising applications in inducing chirality into non-chiral liquid crystal matrices.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Biochemistry & Molecular Biology
Vladyslav Savchenko, Nino Lomadze, Svetlana Santer, Olga Guskova
Summary: This study investigates the molecular and photophysical properties of a spiropyran-containing amphiphilic molecule in organic and aqueous solutions. The results show that the molecule exhibits positive photochromism in organic solvents, but negative photochromism in water. The explanation lies in the stabilization of the merocyanine form in water, which is supported by density functional theory calculations and classical modeling. Molecular dynamics simulations also reveal the self-assembly of merocyanine molecules in water, forming elongated associates with stack-like building blocks.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Chemistry, Multidisciplinary
Zilong Xie, Zhengli Dou, Die Wu, Xiangtong Zeng, Yuan Feng, Yunfei Tian, Qiang Fu, Kai Wu
Summary: Inspired by the bone joint, researchers have developed a polydimethylsiloxane/alumina (PDMS/Al2O3) thermal interface material (TIM) with enhanced rheological mobility and thermal conductivity by incorporating gallium-based liquid metal (LM). The LM reduces the viscosity at the polymer-LM-Al2O3 interface, allowing for high-loading TIMs while maintaining a thixotropic state and reducing contact thermal resistance. Additionally, the merging of LM droplets bridges separate Al2O3 particles, improving interfacial thermal conduction and enhancing thermal conductivity.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Kirill Gurdumov, Ursula Mazur, K. W. Hipps
Summary: The growth, dynamics, and stability of a model noncovalent self-assembler, Co(II) octaethylporphyrin, at the solution-HOPG interface were investigated via real-time imaging, scanning tunneling microscopy, and computational methods. The choice of organic solvent was found to play a crucial role in the kinetics and structure of the self-assembled monolayers.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Multidisciplinary Sciences
Thomas G. Parton, Richard M. Parker, Gea T. van de Kerkhof, Aurimas Narkevicius, Johannes S. Haataja, Bruno Frka-Petesic, Silvia Vignolini
Summary: The transfer of chirality across length-scales is an intriguing and universal natural phenomenon, but connecting the properties of individual building blocks to the emergent features of their resulting large-scale structure remains a challenge. In this work, the authors investigate the origins of mesophase chirality in cellulose nanocrystal suspensions, whose self-assembly into chiral photonic films has attracted significant interest.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Peter Knecht, Bodong Zhang, Joachim Reichert, David A. Duncan, Martin Schwarz, Felix Haag, Paul T. P. Ryan, Tien-Lin Lee, Peter S. Deimel, Peter Feulner, Francesco Allegretti, Willi Auwaerter, Guillaume Medard, Ari Paavo Seitsonen, Johannes Barth, Anthoula C. Papageorgiou
Summary: Controlling the arrangement of N-heterocyclic carbenes (NHCs) on solid surfaces is achieved by introducing Ru porphyrins as a control agent, allowing for precise and reversible functionalization on an atomic scale. This arrangement enables the creation of patterned structures on the nanometer scale through controlled manipulation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Multidisciplinary Sciences
Sebastian Echeverria-Alar, Marcel G. Clerc, Ignacio Bordeu
Summary: Spatial branching processes are observed in chiral nematic liquid crystals, where a cholesteric phase self-organizes into extended branching patterns. We study the spatial and temporal organization of thermally driven branching patterns in chiral nematic liquid crystal cells experimentally, and describe the observations using a mean-field model.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Multidisciplinary Sciences
Kyung Sun Park, Zhengyuan Xue, Bijal B. Patel, Hyosung An, Justin J. Kwok, Prapti Kafle, Qian Chen, Diwakar Shukla, Ying Diao
Summary: By studying the assembly process of achiral conjugated polymers, the authors discovered the emergence of chirality and the formation of hierarchical helical structures. This study has significant implications for the development of chiral (opto)electronics.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Katharina Wussow, Andrea Abram, Klaus Koehler, Chun-Ran Chang, Alexander Genest, Jun Li, Notker Roesch
Summary: The relevant parameters for leaching palladium atoms from small Pd clusters during Heck reactions have been studied computationally and experimentally. The results show that bromide ions and other factors make the leaching process notably exergonic.
CATALYSIS COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Renan Villarreal, Pin-Cheng Lin, Zviadi Zarkua, Harsh Bana, Hung-Chieh Tsai, Manuel Auge, Felix Junge, Hans Hofsaess, Ezequiel Tosi, Steven De Feyter, Stefan De Gendt, Steven Brems, E. Harriet ahlgren, Lino M. C. Pereira
Summary: Ultralow energy (ULE) ion implantation is increasingly used to modify 2D materials, in particular, graphene. However, the disorder induced by ion irradiation in this low-energy limit remains poorly understood.
Article
Chemistry, Physical
Ake Andersson, Vasyl Yatsyna, Mathieu Linares, Anouk Rijs, Vitali Zhaunerchyk
Summary: We investigate the gas-phase structure of the neutral pentaalanine peptide using supersonic jet cooling, infrared multiphoton dissociation, and vacuum-ultraviolet action spectroscopy. The molecule assumes multiple stable conformations, mainly of two structure types, with the most stable conformation featuring a C5 ring at the N-terminus and a 310-helix backbone with two beta-turns. The conformational preferences of pentaalanine are also evaluated using Born-Oppenheimer molecular dynamics, revealing a systematic frequency shift caused by a nonzero simulation time step.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Tamara Rinkovec, Demian Kalebic, Mark Van der Auweraer, Wim Dehaen, Jeremy N. Harvey, Steven De Feyter
Summary: In this study, the effect of concentration on the self-assembled molecular network formation process was investigated using scanning tunneling microscopy. Isophthalic acids were chosen as a model system, and the adsorption behavior was evaluated at the nanoscale. The results showed the existence of a critical concentration for self-assembly, with the molecular structure having a significant impact on this threshold value. Furthermore, highly cooperative behavior was observed at the liquid/solid interface, providing a rare example of quantitative measurement of cooperative phenomena.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Yuan Fang, Oleksandr Ivasenko, Ana Sanz-Matias, Kunal S. Mali, Kazukuni Tahara, Yoshito Tobe, Steven De Feyter
Summary: Self-assembled molecular networks (SAMNs) are spontaneously formed through the assembly of molecules on surfaces. Scanning tunneling microscopy (STM) can track their growth dynamics on conductive atomically flat surfaces and at the liquid-solid interface. Desorption and adsorption dynamics are challenging to investigate through the liquid-solid interface. Porous molecular networks have attracted particular interest as they can act as platforms for sensing and host-guest chemistry. However, their stability in a liquid environment is still poorly understood. In this study, the authors investigated the desorption/adsorption dynamics of supramolecular porous monolayers at the interface between highly oriented pyrolytic graphite and 1-phenyloctane, and revealed the time scales, temperature dependence, and the role of STM tip in inducing dynamics.
Article
Chemistry, Physical
Zeno Tessari, Kazukuni Tahara, Steven De Feyter
Summary: When molecules self-assemble on graphene, six orientational domains are usually formed, which can be classified into two sets of packing chirality. Dynamic nanoconfinement conditions disrupt the equivalence of orientational domains and can result in selective formation of enantiomorphic packings. In this study, we investigate the self-assembly of a molecule with four alkyl chains under dynamic nanoconfinement conditions and find biased formation of rotational domains and partial chiral selection. This highlights the significance of using dynamic nanoconfinement conditions to control domain orientation and disturb chirality equivalence.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Gangamallaiah Velpula, Jian Xiang Lian, David Cornil, David Beljonne, Roberto Lazzaroni, Kunal S. Mali, Steven De Feyter
Summary: This study investigates the impact of the anions in imidazolium-based ionic liquids (ILs) on the interface between ILs and graphene, as well as on the electronic structure of graphene. Raman spectroscopy reveals that ILs with smaller anions lead to n-type doping, while ILs with larger anions have a negligible effect on doping. Molecular modeling simulations suggest that changes in the electrostatic potential at the IL-graphene interface are responsible for the n-type doping.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Sota Aoi, Shingo Hirose, Kanagawa Wakana Soeda, Hiromasa Kaneko, Kunal S. Mali, Steven De Feyter, Kazukuni Tahara
Summary: We demonstrate the controlled grafting of graphite surfaces using electrochemically generated aryl radicals templated by self-assembled molecular networks (SAMNs) of bisalkylurea derivatives. The degree of dynamics at the alkyl termini and strong intermolecular interactions play a crucial role in the covalent attachment.
Article
Chemistry, Physical
Nghia Nguyen Thi Minh, Afshan Begum, Jun Zhang, Petter Leira, Yogesh Todarwal, Mathieu Linares, Patrick Norman, Dean Derbyshire, Eleonore von Castelmur, Mikael Lindgren, Per Hammarstroem, Carolin Koenig
Summary: Misfolding and aggregation of transthyretin (TTR) can lead to various amyloid diseases. TTR not only acts as an amyloidogenic protein but also has an affinity for small-molecule ligands in its thyroxine (T4) binding site. In this study, we investigated the binding of a fluorescent amyloid ligand, Py1SA, to tetrameric TTR using spectroscopic evidence and X-ray crystallography. Although the X-ray diffraction data were inconclusive, molecular dynamics simulations and umbrella sampling approaches were used to determine the preferred orientation of the ligand in the T4 binding site. Our findings provide insights into the binding mode preference of TTR for trans-stilbene salicylic acid derivatives and a framework for determining structures of TTR-ligand complexes.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Multidisciplinary
Marina Gonzalez-Sanchez, Mariia J. Mayoral, Violeta Vazquez-Gonzalez, Marketa Paloncyova, Irene Sancho-Casado, Fatima Aparicio, Alberto de Juan, Giovanna Longhi, Patrick Norman, Mathieu Linares, David Gonzalez-Rodriguez
Summary: Self-assembled nanotubes with distinct internal arrangements and properties are achieved through different supramolecular scenarios prior to polymerization, driven by chelate cooperativity and self-recognition motifs at the edges. The chosen supramolecular pathway for structurally related molecules with complementary nucleobases is determined by their propensity for specific cyclic structures through Watson-Crick pairing. These findings provide insight into the unpredictability and experimental evaluation of self-assembly pathways, as well as the design of functional nanomaterials with controlled helicity and chiroptical properties.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Analytical
Jordan C. Potts, Akhil Jain, David B. Amabilino, Frankie J. Rawson, Lluisa Perez-Garcia
Summary: This study presents a new method based on UV-visible absorption spectrum to accurately calculate the concentration and number of molecules bound to multifunctional AuNPs. The method is able to reveal the precise binding situation of Cyt C and Zn Porph molecules with each multifunctional AuNP, providing valuable information for applications in drug delivery and biosensors.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Tamara Rinkovec, Demian Kalebic, Mark Van der Auweraer, Wim Dehaen, Jeremy N. Harvey, Steven De Feyter
Summary: This study investigates the effect of concentration on the self-assembly process of molecular networks using scanning tunneling microscopy. The research aims to improve the understanding of 2D supramolecular chemistry by obtaining quantitative data. The results show highly cooperative behavior and the significant impact of molecular structure on the critical concentration.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Michael Clarke, Abigail Bellamy-Carter, Ferdinando Malagreca, Jack Hart, Stephen P. Argent, James N. O'Shea, David B. Amabilino, Alex Saywell
Summary: The incorporation of organic semiconducting materials within solid-state electronic devices is important for highly efficient photovoltaics, transistors, and light emitting diodes. This study focuses on the formation of a polymer based on a diketopyrrolopyrrole (DPP) monomer unit, which is synthesized on a surface and possesses aryl-halide groups for covalent coupling. The self-assembly of both the monomer material and the domains of polymeric material are investigated using scanning tunneling microscopy and X-ray photoelectron spectroscopy.
MOLECULAR SYSTEMS DESIGN & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Yuta Sato, Steven De Feyter, Kazukuni Tahara
Summary: This study reports the formation of porous structures on alkane buffer layers on graphite through molecular self-assembly. Dehydrobenzo[12]-annulene (DBA) derivative was found to form hexagonal structures on n-pentacontane and n-hexacontane buffer layers through van der Waals interactions. The nucleation and structural growth of the DBA network on a buffer layer were discussed, and a hierarchical multicomponent structure was formed through heteromolecular coadsorption. This study provides insights into the construction of intricate 3D nanoarchitectures using self-assembly at interfaces.
Article
Chemistry, Multidisciplinary
Matsuhiro Maeda, Kazuya Sato, Steven De Feyter, Kazukuni Tahara
Summary: We report the construction of homochiral, hierarchical self-assembled molecular networks at the liquid/graphite interface using a single chiral molecular building block through dynamic self-sorting.
Article
Materials Science, Multidisciplinary
Zhongnan Duan, Joseph Phillips, Letizia Liiro-Peluso, Simon Woodward, Oleg Makarovsky, Michael P. Weir, H. Jessica Pereira, David B. Amabilino
Summary: The preparation and properties of conducting polymers comprising poly(3,4-ethylenedioxythiophene) (PEDOT) and carrageenan are described. The aim is to provide alternative and sustainable materials that can complement existing conducting polymers. The materials were prepared using chemical oxidation and show good conductivity and thermoelectric properties.
MATERIALS ADVANCES
(2023)