Article
Chemistry, Multidisciplinary
Manuel R. Uhlig, Simone Benaglia, Ravindra Thakkar, Jeffrey Comer, Ricardo Garcia
Summary: Hydration layers form on hydrophilic and hydrophobic crystalline surfaces, but on hydrophobic surfaces, water molecules are expelled and replaced by hydrocarbon molecules near the surface, creating a new interfacial layer.
Article
Chemistry, Physical
E. Nakouzi, S. Kerisit, B. A. Legg, S. Yadav, D. Li, A. G. Stack, C. J. Mundy, J. Chun, G. K. Schenter, J. J. De Yoreo
Summary: Solid-liquid interfaces play a crucial role in various phenomena such as colloidal aggregation, crystallization, catalysis, nucleation, water desalination, and biomolecular assembly. This study investigates the influence of hydrophilic and hydrophobic probes on interfacial solution structure using three-dimensional atomic force microscopy (3D AFM). The results show that hydrophilic probes exhibit good agreement with molecular dynamics simulations, while hydrophobic probes detect vertical oscillatory features without matching the underlying lattice. It is also found that the repulsive hydration force between the probe and mica depends on the nature and concentration of ions in the solution. Based on these findings, a scheme for controlling particle aggregation and attachment outcomes by tuning hydration force is proposed.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Yi-Feng Wang, Yi-Bo Wang, Xin He, Ben-Xi Zhang, Yan-Ru Yang, Xiao-Dong Wang, Duu-Jong Lee
Summary: This study investigates the retraction dynamics of low-viscosity water nanodroplets on different surfaces through molecular dynamics simulations. Two retraction regimes, inertial and capillary regimes, are defined, and the retraction velocities are found to depend on the impact velocity and surface wettability.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Thermodynamics
Mustafa Sengul, Esra H. Isik, I. Bedii Ozdemir
Summary: The study compared a new hybrid dynamic contact angle approach with four other models in investigating water droplet flows on surfaces, finding the hybrid model to be the most successful. Results suggest that the motion of droplets is highly dependent on the formulation of the dynamic contact angle in relation to surface wettability, with the hybrid model being successful on both hydrophobic and hydrophilic surfaces.
HEAT TRANSFER ENGINEERING
(2022)
Article
Thermodynamics
Zhibing Zhu, Xuan Zhang, Yugang Zhao, Xiaoyang Huang, Chun Yang
Summary: The freezing characteristics of deposited water droplets on aluminum surfaces were investigated experimentally and theoretically compared with those of sessile droplets. The results showed differences in freezing behavior and frozen shapes between deposited and sessile droplets, depending on surface temperature and wettability.
INTERNATIONAL JOURNAL OF THERMAL SCIENCES
(2022)
Article
Biochemistry & Molecular Biology
Francesco Mallamace, Domenico Mallamace, Sow-Hsin Chen, Paola Lanzafame, Georgia Papanikolaou
Summary: NMR spectroscopy was used to study the competition of hydrophobic effects in solutions of water with glycerol and methanol, revealing different behaviors of studied quantities under various conditions. Liquid water properties are dominated by hydrogen bond interactions, with a focus on the hydrophobic effects of these structures.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2021)
Article
Chemistry, Physical
Fabio Staniscia, Horacio Guzman, Matej Kanduc
Summary: This study investigates the adsorption behavior of short-chained alcohols to water-vapor interfaces and solid surfaces with different polarities using molecular dynamics simulations. The researchers derive an equation for the adsorption coefficient, which shows exponential dependence on both molecular surface area and surface wetting coefficient. The findings suggest that the influence of surfactants on sessile droplets is strongest on highly hydrophilic and hydrophobic surfaces, while moderately hydrophilic surfaces are less affected.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Applied
Piotr Krol, Monika Szlachta, Kinga Pielichowska
Summary: Polyurethane cationomers thin films with surface functionalized TiO2 as ecological water dispersions were obtained, showing considerable changes in thermal, mechanical, and surface properties. Films made with MDI isocyanate surface-modified TiO2 were hydrophobic, while those with unmodified TiO2 were hydrophilic. The enhanced thermal and mechanical properties make these cationomers promising for modern coating materials.
PROGRESS IN ORGANIC COATINGS
(2022)
Article
Materials Science, Multidisciplinary
Luis Humberto Robledo-Taboada, Javier Francisco Jimenez-Jarquin, Fernando Chinas-Castillo, Antonio Mendez-Blas, Santiago Camacho-Lopez, Laura Elvira Serrano-de La Rosa, Magdaleno Caballero-Caballero, Rafael Alavez-Ramirez, Martha Hilaria Bartolo-Aleman, Efren Normando Enriquez-Porras
Summary: This study investigated the effects of surface texturing on friction and wear using different current levels to anodize p-type silicon samples. The results showed that low currents generated mesoporous silicon surfaces with low friction, while high currents generated macroporous silicon surfaces with high friction. The study also revealed a direct correlation between pore size and wear volume, as well as scar diameter.
JOURNAL OF MATERIALS RESEARCH AND TECHNOLOGY-JMR&T
(2022)
Article
Polymer Science
Junsu Park, Yuki Shimizu, Xin Zhou, Ryohei Ikura, Go Matsuba, Yoshinori Takashima
Summary: Photoresponsiveness is a promising characteristic of stimulus-responsive materials, which can be achieved by incorporating photoresponsive molecules into polymeric materials. Moisture- and photoresponsive materials, the focus of this report, exhibit bending behaviors at different water contents and their switching behavior can inspire strategies for the application of polymeric materials as actuators.
Article
Chemistry, Physical
Justin Engstler, Nicolas Giovambattista
Summary: Water-mediated interactions play important roles in aqueous solutions, affecting processes such as protein folding and nanoparticle aggregation. This study investigates the impact of temperature and pressure on different types of interactions between graphene-based surfaces. The results show that hydrophobic, hydrophilic, and hybrid interactions are all sensitive to pressure, while only hydrophobic interactions are significantly affected by temperature variations. The findings have implications for understanding protein denaturation and biomolecular interactions, as well as for the design of water models for molecular and nanoparticle systems under different thermodynamic conditions.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Farzin Saffarimiandoab, Roozbeh Sabetvand, Xihui Zhang
Summary: This study investigates various desalination mechanisms of capacitive deionization (CDI) systems and their relationship with performance. The results show that the microscopic properties of the confined electrolytes directly influence the water cluster structure and desalination performance. Additionally, factors such as ionic species solvation structure, capacitance, and charge efficiency are found to have complex relationships with desalination capacity.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Nanoscience & Nanotechnology
Zhen Qin, Hang Sun, Yanan Tang, Shengyan Yin, Lixue Yang, Mingwei Xu, Zhenning Liu
Summary: A bioinspired hydrophilic-hydrophobic Janus hybrid system was constructed for efficient solar steam generation and water evaporation, with the added benefit of effective sewage purification.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Rui Zhao, Meng Yu, Zhe Sun, Shou-he Pan, Yin-min Wang, Ying-jian Ma, Xin-yu Guo, Yong Xu, Xue-min Wu
Summary: The length of the hydrophilic chain in nonionic surfactants has an impact on the regulation of droplet impact behavior and wetting behavior on hydrophobic surfaces. Longer hydrophilic chains lead to better regulation of droplet impact behavior and suppression of droplet rebound, while shorter hydrophilic chains lead to better regulation of droplet wetting behavior. These findings contribute to a better understanding of the mechanism behind regulating droplet behavior and surfactant solution wetting on hydrophobic surfaces.
SURFACES AND INTERFACES
(2023)
Article
Chemistry, Physical
Shohei Ida, Daiki Nishisako, Ayaka Fujiseki, Shokyoku Kanaoka
Summary: Thermoresponsive hydrogels synthesized via free radical copolymerization can achieve sharp volume changes upon heating, with gels containing hydrophobic acrylamide monomers exhibiting significant responsiveness. The formation of a local amphiphilic structure is crucial for achieving sharp thermoresponsiveness.
Article
Chemistry, Physical
Ali Eltareb, Gustavo E. Lopez, Nicolas Giovambattista
Summary: In this study, path integral molecular dynamics simulations were used to investigate a monatomic liquid with a liquid-liquid phase transition and critical point. By varying Planck's constant, the researchers were able to observe the effects of nuclear quantum effects on the liquid's behavior. The simulations, combined with ring-polymer molecular dynamics, revealed anomalous glass transition temperatures and a pressure-induced transformation between low-density and high-density amorphous ice.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Thomas E. Gartner, Kelly M. Hunte, Eleftherios Lambros, Alessandro Caruso, Marc Riera, Gregory R. Medders, Athanassios Z. Panagiotopoulos, Pablo G. Debenedetti, Francesco Paesani
Summary: In this study, molecular dynamics simulations with the many-body MB-pol model were used to investigate the thermodynamic response and local structure of liquid water at different temperatures. The results suggest that the MB-pol model has predictive capability for the physical properties of liquid water across a wide range of thermodynamic states, including the difficult-to-probe "water's no man's land."
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Jack Weis, Francesco Sciortino, Athanassios Z. Panagiotopoulos, Pablo G. Debenedetti
Summary: Recent experiments and numerical simulations have provided support to the hypothesis that a second critical point exists in deeply supercooled water. In particular, a study has found that a liquid-liquid critical point can be located using a model parameterized solely based on ab initio calculations. This finding is important for understanding the phase behavior of supercooled water.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Yiming Wang, Frank H. Stillinger, Pablo G. Debenedetti
Summary: In this study, molecular dynamics simulations were performed to investigate the fluid-fluid phase transitions of a flexible three-dimensional four-site chiral molecular model. By introducing bias favoring local homochiral vs heterochiral interactions, the system exhibited a phase transition from a single achiral phase to a single chiral phase, with infrequent interconversion between the two chiral states. The results provide basic thermodynamic and kinetic insights for understanding many-body chiral symmetry breaking phenomena.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Justin Engstler, Nicolas Giovambattista
Summary: Water-mediated interactions play important roles in aqueous solutions, affecting processes such as protein folding and nanoparticle aggregation. This study investigates the impact of temperature and pressure on different types of interactions between graphene-based surfaces. The results show that hydrophobic, hydrophilic, and hybrid interactions are all sensitive to pressure, while only hydrophobic interactions are significantly affected by temperature variations. The findings have implications for understanding protein denaturation and biomolecular interactions, as well as for the design of water models for molecular and nanoparticle systems under different thermodynamic conditions.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Multidisciplinary Sciences
Pablo M. Piaggi, Jack Weis, Athanassios Z. Panagiotopoulos, Pablo G. Debenedetti, Roberto Car
Summary: Molecular simulations based on machine-learning models and density-functional theory have provided insights into the mechanism of homogeneous ice nucleation. The results are in good agreement with experimental measurements, and the impact of factors such as thermodynamic driving force, interfacial free energy, and stacking disorder on nucleation rates has been studied.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Physical
Yang Zhou, Gustavo E. E. Lopez, Nicolas Giovambattista
Summary: As a liquid approaches the gas state, the properties of the potential energy landscape sampled by the system become anomalous. Cavitation and spinodal-like minimum in pressure are observed, and at intermediate/high temperatures, crystallization of the liquid can occur. The liquid-liquid phase transition also exhibits heterogeneous properties.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Nikolai D. Petsev, Arash Nikoubashman, Folarin Latinwo, Frank H. Stillinger, Pablo G. Debenedetti
Summary: Chiral crystals and their constituent molecules are important in theories about the origin of biological homochirality and in drug discovery, design, and stability. The prediction and identification of stable chiral crystal structures is complicated by many body interactions and molecular complexity. This study uses genetic algorithms to predict crystal lattices formed by a chiral tetramer molecular model and explores the stability and structures of conglomerate and racemic crystals.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Physics, Multidisciplinary
Thomas E. Gartner III, Pablo M. Piaggi, Roberto Car, Athanassios Z. Panagiotopoulos, Pablo G. Debenedetti
Summary: The study provides preliminary evidence of liquid-liquid phase transition in water using molecular simulation techniques and a neural network model based on density functional theory calculations.
PHYSICAL REVIEW LETTERS
(2022)
Article
Multidisciplinary Sciences
Thomas J. Longo, Nikolay A. Shumovskyi, Betul Uralcanc, Sergey. V. V. Buldyrev, Mikhail A. Anisimov, Pablo G. Debenedetti
Summary: The separation of substances into different phases is a common and important phenomenon in nature and has scientific and technological significance. When the species involved can interconvert, the presence of a strong external force can result in equal amounts of both alternative species and the observation of steady-state, restricted phase separation. This study uses simulations to investigate the formation of such mesoscale steady-state structures in binary mixtures that exhibit both equilibrium and forced interconversion, and shows that a nonequilibrium thermodynamic theory can explain the main trends and observations.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Multidisciplinary Sciences
Katrin Amann-Winkel, Kyung Hwan Kim, Nicolas Giovambattista, Marjorie Ladd-Parada, Alexander Spaeh, Fivos Perakis, Harshad Pathak, Cheolhee Yang, Tobias Eklund, Thomas J. Lane, Seonju You, Sangmin Jeong, Jae Hyuk Lee, Intae Eom, Minseok Kim, Jaeku Park, Sae Hwan Chun, Peter H. Poole, Anders Nilsson
Summary: Recent experiments have provided evidence for a liquid-liquid phase transition (LLPT) in supercooled water, which can explain the anomalous properties of liquid water and amorphous ice. By subjecting low-density amorphous (LDA) ice to ultrafast heating, researchers observed the coexistence of high-density and low-density liquid phases, and confirmed the LLPT using femtosecond x-ray laser pulses.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Ali Eltareb, Gustavo E. E. Lopez, Nicolas Giovambattista
Summary: In this study, we use PIMD and classical MD simulations to investigate the nuclear quantum effects (NQE) on the thermodynamic properties of low-density amorphous ice (LDA) and hexagonal ice (I(h)). Our results demonstrate that including NQE is crucial to accurately reproduce the experimental properties of LDA and ice I(h). While MD simulations (without NQE) indicate a monotonic increase in the density ρ-(T) of LDA and ice I(h) upon cooling, PIMD simulations show the presence of a density maximum. Additionally, MD and PIMD simulations suggest different temperature dependences for the thermal expansion coefficient α(P)(T) and bulk modulus B(T) of both LDA and ice I(h).
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Physical
Pablo M. Piaggi, Roberto Car, Frank H. Stillinger, Pablo G. Debenedetti
Summary: Understanding the behavior of chiral molecules in condensed phase is crucial for biology and various technological applications. In this study, molecular dynamics simulations were used to investigate a chiral molecular model with second-order symmetry-breaking phase transition and determine the critical temperature. The finite-size scaling behavior of the order parameter suggests compatibility with the 3D Ising universality class. The presence of a free energy barrier indicates a suppressed fluctuation between the enantiomers, which could explain the origin of biological homochirality.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Pablo M. Piaggi, Thomas E. Gartner III, Roberto Car, Pablo G. Debenedetti
Summary: The possible existence of a liquid-liquid critical point in deeply supercooled water has been debated. Mishima and Stanley studied the melting curves of different ice polymorphs and suggested that the critical point lies between the melting curves of ice III and ice V. However, our molecular dynamics simulations and machine learning model based on ab initio calculations show that the melting curves of ices III, IV, V, VI, and XIII are supercritical and do not intersect the liquid-liquid transition locus. We conclude that the scenario in which the melting curves are supercritical is favored by the most recent computational and experimental evidence.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Binze Tang, Sergey V. Buldyrev, Limei Xu, Nicolas Giovambattista
Summary: Nanoscale water capillary bridges (WCB) formed between patchy surfaces can extract energy from the environment by responding to changes in relative humidity (RH). The energy density extracted by the nanoscale WCB is approximately 1700 kJ/m(3), comparable to other water-responsive materials.