Article
Chemistry, Multidisciplinary
Olivia P. L. Dalby, Steven Abbott, Nobuyuki Matubayasi, Seishi Shimizu
Summary: In this paper, we propose a statistical thermodynamic approach to model stepwise isotherms in heterogeneous adsorbents. Our approach, based on rigorous statistical thermodynamic theory, avoids unrealistic assumptions and limitations of previous models. It provides a universal method for modeling different types of adsorbents and offers clear insights into sorption mechanisms.
Article
Chemistry, Multidisciplinary
Chunhui Zhang, Xiao Xiao, Ziwei Guo, Lei Jiang, Cunming Yu
Summary: Researchers have investigated the formation, transportation, and spreading of bubbles on solid surfaces with specific wettability. However, bubble transfer on wettability-heterogeneous surfaces has been rarely reported. This study investigates the behavior of bubble transfer on such surfaces and explores their application in micro-bubble collection and H-2 bubble removal in water splitting.
CHINESE CHEMICAL LETTERS
(2023)
Article
Engineering, Environmental
Akash Raman, Carla Corina dos Santos Porto, Han Gardeniers, Cintia Soares, David Fernandez Rivas, Natan Padoin
Summary: This study simulated a system consisting of spatially-decoupled electrolytic bubbles and analyzed the growth and departure process of electrolytic bubbles and their impact on gas evolution efficiency.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Thermodynamics
S. Y. Misyura, V. S. Morozov, R. Egorov
Summary: Experimental studies are conducted to investigate the non-isothermal evaporation and heat transfer of water droplets and films on structured walls. The results show that the textured surfaces can change the wettability and enhance the heat transfer, leading to an increased evaporation rate. Furthermore, self-organization of colloidal aqueous solution films under local heating is observed.
INTERNATIONAL JOURNAL OF HEAT AND MASS TRANSFER
(2022)
Article
Energy & Fuels
Sohaib Mohammed, Hassnain Asgar, Chris J. Benmore, Greeshma Gadikota
Summary: This study explores the crystallization onset and growth of confined benzene in nanopores and reveals that the crystallization temperature of confined benzene is lower than that of bulk benzene. The crystals initiate on the pore surface and grow towards the pore center. Additionally, the dynamics behavior of confined benzene undergoes a transition from fragile to strong dynamics. These findings have significant implications for understanding the phase behavior of confined organic liquids and their applications in various fields.
Article
Engineering, Multidisciplinary
Chunjin Wang, Zili Zhang, Chi Fai Cheung, Wang Luo, Yee Man Loh, Yanjun Lu, Lingbao Kong, Shixiang Wang
Summary: This paper presents a novel maskless fluid jet polishing (MFJP) technique to improve the quality of optical structured surfaces, and experimental investigations demonstrate its technical feasibility on sinusoidal and V-groove structures. The results indicate that MFJP can significantly enhance the surface quality of optical structured surface and possess high form maintainability under certain conditions.
PRECISION ENGINEERING-JOURNAL OF THE INTERNATIONAL SOCIETIES FOR PRECISION ENGINEERING AND NANOTECHNOLOGY
(2022)
Article
Materials Science, Multidisciplinary
Yu Liang, Bo-Han Li, Ziling Li, Guanhua Zhang, Julong Sun, Chuanyao Zhou, Youtian Tao, Yu Ye, Zefeng Ren, Xueming Yang
Summary: This study investigated the ultrafast carrier dynamics of two-dimensional molybdenum disulfide (MoS2) flakes using femtosecond time-resolved micro-area photoelectron spectroscopy and photoemission electron microscopy. Spatial heterogeneity and defect effects were observed, with defects significantly shortening charge carrier lifetime while acting as recombination centers. Three relaxation processes were identified in the photoelectron intensity dynamics, with different rates influenced by defect density and bulk electron transportation. The results deepen the understanding of interfacial carrier dynamics and defect effects on charge carrier lifetime in MoS2 materials.
MATERIALS TODAY PHYSICS
(2021)
Article
Mathematics, Applied
M. Mohasan, A. B. Aqeel, Huiling Duan, Pengyu Lyu, Yantao Yang
Summary: This study numerically investigates the impact of droplets on a thin liquid film deposited on a structured surface. The results show that the surface structure has a significant effect on the crown height and radius of the droplets, and can prevent the droplets from breaking into satellite droplets.
APPLIED MATHEMATICS AND MECHANICS-ENGLISH EDITION
(2022)
Article
Chemistry, Physical
Zhen Ye, Masayoshi Mizutani
Summary: This study presents a new method to predict the apparent contact angle on structured surfaces by utilizing the properties of the actual contact angle. Experiments confirm the validity of the proposed model, showing that the apparent contact angle is influenced only by the material at the triple contact line and remains independent of the contact area. The Wenzel equation is deemed inadequate for calculating the apparent contact angle on most structured surfaces.
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
(2023)
Article
Multidisciplinary Sciences
Jiaqi Li, Daniel Kang, Kazi Fazle Rabbi, Wuchen Fu, Xiao Yan, Xiaolong Fang, Liwu Fan, Nenad Miljkovic
Summary: This study used high-magnification in-liquid endoscopy to investigate bubble behavior during boiling on structured surfaces, revealing the previously unknown coexistence of two distinct three-phase contact lines, resulting in the retention of a thin liquid film between the two contact lines. This finding sheds light on a previously unidentified mechanism governing bubble evolution on structured surfaces and has significant implications for various real systems utilizing bubble formation.
Article
Materials Science, Multidisciplinary
Hyeonho Cho, Do-Nyun Kim
Summary: The art of kirigami has provided a versatile way to construct reconfigurable structures. This study focuses on controlling the stiffness of bistable kirigami surfaces while maintaining the target 3D shape. A computational procedure is developed to design various bistable kirigami surfaces, and its predictions are validated through experiments. The study finds that the range of stiffness for deployed bistable kirigami surfaces can be significantly broadened by using spatially varying hinges without altering the shape and stability.
MATERIALS & DESIGN
(2023)
Article
Thermodynamics
Hai Wang, Fan Zhang, Junfeng Wang, Zhentao Wang, Haojie Xu, Wei Zhang
Summary: The frosting behavior and dynamic defrosting characteristics of horizontally oriented hybrid surfaces with heterogeneous wettability were investigated in this study. The developed hybrid surfaces integrated the properties of frost retardation and fast surface cleaning upon defrosting. Hybrid surfaces exhibited superior anti-frosting performance compared to a bare copper surface but not as good as a complete superhydrophobic surface. Surface energy gradient and Laplace pressure gradient enabled by heterogeneous wettability on hybrid surfaces facilitated quick cleaning during the defrosting process. The proportion of surface clean time on hybrid surfaces was as low as 32.2%-41.5% of one full cycle duration.
CASE STUDIES IN THERMAL ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Xifan Fu, Qinpeng Zhu, Denghui Liu, Binghan Liu, Lintao Kuang, Yanhui Feng, Fuqiang Chu, Zhi Huang
Summary: A study on moisture condensation on hybrid superhydrophobic-hydrophilic surfaces revealed the significant impact of wettability difference and microstructure size on condensation efficiency, leading to a 90% enhancement in condensation rate. Detailed analysis of the condensation process provided insights into the enhanced condensation mechanism, proposing effective methods for controlling and optimizing moisture condensation.
Article
Chemistry, Multidisciplinary
Jean-Francois Bryche, Marlo Vega, Agnes Tempez, Thibault Brule, Thomas Carlier, Julien Moreau, Marc Chaigneau, Paul G. Charette, Michael Canva
Summary: This work demonstrates the enhancement in plasmonic sensing efficacy by spatially-localized functionalization on nanostructured surfaces, where probe molecules are concentrated in areas of high field concentration. SERS measurements on nanostructured surfaces with homogeneous and spatially-localized functionalization with thiophenol show that the Raman signal mainly originates from high field concentration areas. TERS measurements with 10 nm spatial resolution confirm the predicted field distribution profiles.
Review
Chemistry, Physical
Xiaogang Yang, Yuanxing Wang, Chang Ming Li, Dunwei Wang
Summary: This review summarizes current advances in studies on surface chemistry within the context of water oxidation, including intermediates, reaction mechanisms, and their influences on the reaction kinetics. It also outlines how multiple charge transfer relies on intermediate coverage and accumulated charge numbers. Density functional theories are used to discuss intermediates and rate-determining steps on some water oxidation catalysts.
Article
Chemistry, Physical
V. Conti Nibali, S. Pezzotti, F. Sebastiani, D. R. Galimberti, G. Schwaab, M. Heyden, M-P Gaigeot, M. Havenith
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2020)
Article
Physics, Fluids & Plasmas
Julius C. F. Schulz, Alexander Schlaich, Matthias Heyden, Roland R. Netz, Julian Kappler
PHYSICAL REVIEW FLUIDS
(2020)
Article
Biochemistry & Molecular Biology
Yanxian Lin, Yann Fichou, Andrew P. Longhini, Luana C. Llanes, Pengyi Yin, Guillermo C. Bazan, Kenneth S. Kosik, Songi Han
Summary: The liquid-liquid phase separation of tau protein can facilitate amyloid aggregation in some cases, while being independent of aggregation in others. The nature of the interaction driving tau condensation is a differentiating factor between aggregation-prone and aggregation-independent liquid-liquid phase separations.
JOURNAL OF MOLECULAR BIOLOGY
(2021)
Article
Chemistry, Physical
Matthias Heyden, Dmitry Matyushov
JOURNAL OF PHYSICAL CHEMISTRY B
(2020)
Article
Physics, Multidisciplinary
Giorgio Schiro, Yann Fichou, Alex P. S. Brogan, Richard Sessions, Wiebke Lohstroh, Michaela Zamponi, Gerald J. Schneider, Francois-Xavier Gallat, Alessandro Paciaroni, Douglas J. Tobias, Adam Perriman, Martin Weik
Summary: The study revealed that solvent-free protein-polymer hybrids can replace hydration water, preserving protein structure and function, with dynamics similar to water's.
PHYSICAL REVIEW LETTERS
(2021)
Article
Chemistry, Physical
Tawny N. Fajardo, Matthias Heyden
Summary: By analyzing the free energy surface of a small peptide, individual contributions that stabilize or destabilize compact and extended peptide conformations can be identified, shedding light on the origin of the free energy barrier associated with transitions between different conformations.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Biochemical Research Methods
Morteza M. Waskasi, Aleksandar Lazaric, Matthias Heyden
Summary: DEP is a method used to manipulate micrometer-sized particles, with little effect predicted for nanometer-sized proteins. This study uses molecular dynamics simulations to examine solvent-mediated dielectrophoretic forces on proteins, revealing the potential significance of solvent-mediated contributions to negative protein DEP forces for larger protein structures and high electric field frequencies.
Article
Multidisciplinary Sciences
Kevin Pounot, Markus Appel, Christian Beck, Martin Weik, Giorgio Schiro, Yann Fichou, Tilo Seydel, Frank Schreiber
Summary: Neutron scattering is a nondestructive method for probing the dynamics within samples. This paper presents the workflow and data analysis procedure for investigating protein and hydration water dynamics using neutron backscattering spectroscopy. Two case studies on amyloid proteins are presented to illustrate the method's capability. The importance of neutron scattering in studying dynamics in comparison to other biophysical methods is also discussed.
JOVE-JOURNAL OF VISUALIZED EXPERIMENTS
(2022)
Article
Chemistry, Physical
David Talaga, Gary S. Cooney, Vicky Ury-Thiery, Yann Fichou, Yuhan Huang, Sophie Lecomte, Sebastien Bonhommeau
Summary: Total internal reflection tip-enhanced Raman spectroscopy (TIR-TERS) is a promising technique for noninvasive nanoscale chemical characterization of biomolecules. The TERS enhancement achieved in this configuration is significantly higher than that in traditional illumination geometry. TIR-TERS is applied to the study of Tau amyloid fibrils, revealing spectral signatures and structural information of the fibrils.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Physical
Zhikai Zeng, Yann Fichou, Michael Vigers, Karen Tsay, Songi Han
Summary: The aggregation of tau protein is crucial for tauopathies, and cryogenic electron microscopy has provided high-resolution images of pathological tau tangles. Seeded aggregation is believed to play a significant role in the structural propagation of tau fibrils, but direct measurement of structural evolution is currently lacking. Double electron-electron resonance (DEER) holds unique potential to track the structural changes of tau during aggregation and elucidate disease-specific tau aggregation pathways.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Physical
Valeria Conti Nibali, Sthitadhi Maiti, Franz Saija, Matthias Heyden, Giuseppe Cassone
Summary: Externally applied electric fields in liquid water can induce various effects, but the effects on the total and local entropy of water have not been reported yet. Classic and first-principles molecular dynamics simulations were performed to investigate the entropic contributions of different field intensities in liquid water. The results show that strong fields can align molecular dipoles, but the entropy reductions are modest in classical simulations. The entropy modifications are small even at intense fields, suggesting that electric-field-induced crystallization cannot occur in bulk water at room temperature.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Aleksandar Lazaric, Viren Pattni, Kaprao Fuegner, Arieh Ben-Naim, Matthias Heyden
Summary: In this study, the solvation free energy of benzene derivatives in water was analyzed to guide the development of predictive models for solvation free energies and solvent-mediated interactions. Through spatially resolved analysis and solvation free energy arithmetic, additive models were constructed to describe the solvation of complex compounds. The nonadditive solvation free energy contributions were primarily attributed to electrostatics, which were qualitatively reproduced using computationally efficient continuum models. This study suggests a promising approach for developing efficient and accurate solvation models for complex molecules with varying substitution patterns using solvation arithmetic.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Michael A. Sauer, Matthias Heyden
Summary: This paper introduces a fully anharmonic analysis method for molecular vibrations based on a time correlation formalism, eliminating the need for harmonic or quasi-harmonic approximations. Through molecular dynamics simulations, this new approach can accurately identify the collective degrees of freedom associated with molecular vibrations at any given frequency, unambiguously characterizing the anharmonic nature of low-frequency vibrations in the far-infrared spectrum.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Sthitadhi Maiti, Matthias Heyden
Summary: There is an imbalance between intra-protein and protein-water interactions in many empirical force fields, leading to discrepancies between explicit solvent simulations of intrinsically disordered proteins and experiments. Various strategies have been proposed to modify protein-water interactions and improve agreement with experiments. This study combines simulations with standard and modified force fields and analyzes the solvation free energy contributions to compare the consequences of each strategy. The results show that different strategies have qualitatively different effects on protein solvation, which may affect the protein's tendency to form aggregates or phase-separated droplets, but are not necessarily reflected in comparisons to global parameters.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Physical
Christopher Paslack, Lars Schafer, Matthias Heyden
Summary: This study used molecular dynamics simulations to investigate how internal protein motions and their coupling to the surrounding solvent impact the dynamics of ligand binding to biomolecular surfaces. The results showed that protein flexibility modulates water density fluctuations near the hydrophobic surface patch, smoothing out the friction profile of ligand binding. Internal protein motions were found to shape the effects of enhanced friction in the vicinity of the protein, similar to idealized hydrophobic surfaces.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)