Article
Chemistry, Physical
Zihao Jiao, Mengmeng Song, Ya Liu, Liejin Guo
Summary: Supercritical water is essential in technology and geology. Developing accurate water potential models at the atomic level is crucial, but the rigid model has limitations due to intense vibrations of water molecules in the supercritical region. This study investigates the performance improvement of introducing flexibility in the SPC/Fw model. Molecular dynamics simulations under different thermodynamic conditions reveal that flexibility affects the density, self-diffusion coefficient, and solvation shell of water. The relationship between water geometry, density, averaged H-bond number, and self-diffusion coefficient is established.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Chemistry, Physical
Aigerim Karina, Tobias Eklund, Christina M. Tonauer, Hailong Li, Thomas Loerting, Katrin Amann-Winkel
Summary: High-density amorphous ice (HDA) and low-density amorphous ice (LDA) are counterparts of the high-density and low-density liquid phases of water, respectively. In this study, infrared spectroscopy measurements were conducted to investigate how the vibrational modes change during the transition between HDA and LDA. The results showed a redshift and a drastic decrease in bandwidth from HDA to LDA. The stronger hydrogen bonds in LDA were attributed to changes in coordination number and water molecule interstitials between the first and second hydration shell. Additionally, the unusually broad uncoupled OD band distinguished HDA from other crystalline high-pressure phases.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Multidisciplinary Sciences
Hiromasa Niinomi, Tomoya Yamazaki, Hiroki Nada, Tetsuya Hama, Akira Kouchi, Tomoya Oshikiri, Masaru Nakagawa, Yuki Kimura
Summary: Experimental evidence has been provided for the existence of an unknown water at the ice V-water interface, which is immiscible with the surrounding water. The dewetting dynamics of this unknown water resembles spinodal-like behavior, with a characteristic velocity of approximately 90 m/s. The time evolution of the characteristic length of the spinodal-like undulation suggests that the dynamics can be described using a common model for spinodal decomposition of an immiscible liquid mixture, and the unknown water transiently exhibits anisotropy, indicating liquid crystal properties.
SCIENTIFIC REPORTS
(2023)
Article
Chemistry, Physical
Thaciana Malaspina, Iuliia V. Voroshylova, M. Natalia D. S. Cordeiro, Eudes Eterno Fileti
Summary: This study investigates the structural and spectroscopic properties of amino acid ionic liquids through ab initio molecular dynamics simulations, and provides a comprehensive analysis of the differences between pure and aqueous electrolytes. The findings have important implications for further advancements in the field.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Chemistry, Multidisciplinary
Lee T. Birchall, Amber T. Raja, Lewis Jackson, Helena J. Shepherd
Summary: To improve strategies for spin-crossover material design, obtaining isostructural materials is crucial for developing and understanding structure-property relationships. In this study, we synthesized four isostructural cocrystal solvates using a specific complex and coformer. The spin-crossover properties of these materials were determined by single-crystal X-ray diffraction and were found to be influenced by the hydrogen bond basicity of the anions and solvents present.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Geochemistry & Geophysics
Fei Wang, Elizabeth C. Thompson, Dongzhou Zhang, Jingui Xu, Ercan E. Alp, Steven D. Jacobsen
Summary: This study investigates the deformation and hydrogen bonding structure of Wadsleyite crystal under high pressures, finding that pressure can affect crystal symmetry and structure distortion, as well as the length of the primary hydrogen bond. The primary O1-H hydrogen bond in Wadsleyite becomes highly nonlinear at high pressures.
AMERICAN MINERALOGIST
(2023)
Article
Chemistry, Inorganic & Nuclear
Jack Thomas-Colwell, Arvin Sookezian, Daniel A. Kurtz, Jeremy Kallick, Lawrence M. Henling, Troy A. Stich, Michael G. Hill, Bryan M. Hunter
Summary: We report the isolation and characterization of a series of cobalt(II) bis(phosphine) complexes with varying numbers of coordinated solvent ligands. Comparison of their structures revealed multiple crystallization motifs for divalent cobalt(II) complexes with the same set of phosphine ligands. This study provides a strategy for tuning the axial variability of other ligands on a phosphine scaffold, and proposes a method for designing cobalt phosphine catalysts.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Soon Teh, Po-Jen Hsu, Jer-Lai Kuo
Summary: This study integrated QCE with a molecular-dynamics-based structural searching scheme to investigate cluster sizes in liquid methanol. The analysis revealed that octamer structures significantly contribute to cluster probability, with favorable vibrational free energy playing a key role in making the octamer the dominant species.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Seho Sun, Gaeun Kim, Dongsoo Lee, Eunkyung Park, Seungcheol Myeong, Byoungkuk Son, Kangchun Lee, Minchul Jang, Ungyu Paik, Taeseup Song
Summary: Solvation sheath of Li+-glyme can be adjusted to enhance Li+-TFSI- association, which affects the composition of the solid electrolyte interface (SEI) layer. The formation of TFSI- anion-derived SEI layer on Li metal anode improves Li metal anode efficiency.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Nicolas A. Loubet, Alejandro R. Verde, Jano A. Lockhart, Gustavo A. Appignanesi
Summary: Recent studies have confirmed the existence of a liquid-liquid critical point in numerical models of water. To properly characterize the different molecular arrangements, accurate structural indicators are needed. This study aims to investigate the effect of local structural constraints on water molecules in order to discriminate the different arrangements and develop a multi-molecule structural indicator.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Engineering, Environmental
Wanping Li, Gao Cheng, Shaomin Peng, Ming Sun, Shuzhe Wang, Shengbo Han, Youwen Liu, Tianyou Zhai, Lin Yu
Summary: The study utilized a controllable phosphorization strategy to construct (Fe, Ni)(3)P/NiCoP heterojunction arrays, tuning hydrogen binding energy and demonstrating exceptional Pt-like activity and high stability. This provides a new approach for designing efficient catalytic materials by establishing a clear connection between atomic/interface/electronic structure and intrinsic properties.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Medicinal
Jakub Staron, Wojciech Pietrus, Ryszard Bugno, Rafal Kurczab, Grzegorz Satala, Dawid Warszycki, Tomasz Lenda, Anna Wantuch, Adam S. Hogendorf, Agata Hogendorf, Beata Duszynska, Andrzej J. Bojarski
Summary: The study investigated the binding of fluoxetine and fluvoxamine analogs to SERT, revealing that compounds with heavier halogen atoms bind to SERT through a different binding mode. XSAR analysis showed that E493 and T497 were involved in the formation of the most halogen bonds.
EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
(2021)
Article
Chemistry, Physical
Bo Yang, Hongzhi Lang, Zhe Liu, Shenghan Wang, Zhiwei Men, Chenglin Sun
Summary: Raman spectroscopy was used to investigate the hydrogen bonding network in N, N-dimethylformamide (DMF)-water binary solutions at different mixing ratios. The addition of DMF was found to strengthen the HB network of water when V-DMF is less than 0.4, but destroyed the tetrahedral structure of water at V-DMF of 0.4. Furthermore, DMF-water complexes transformed into DMF center dot H2O structure when V-DMF reached 0.8 due to the instability of DMF center dot nH(2)O (n = 2, 3).
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Chemistry, Multidisciplinary
Li Chen, Jingshuang Dang, Juan Du, Changwei Wang, Yirong Mo
Summary: Recent research has explored the sensitivity of intrinsic bond strengths to external electric fields (EEFs) by examining noncovalent bonds. It was found that X-bonds primarily responded to EEFs due to changes in covalency, while H-bonds were mainly influenced by steric effects. Additionally, X-bonds were more sensitive to EEFs compared to H-bonds, with the key difference lying in charge transfer interactions. Phenylboronic acid was studied as a smart linker in EEFs, demonstrating switchable sensitivity in response to EEFs.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Physical
Marcos Calegari F. Andrade, Tuan Anh Pham
Summary: In this work, large-scale molecular dynamics simulations and machine learning potential derived from first-principles calculations were used to study the hydrogen bonding of water confined in carbon nanotubes (CNTs). The confinement effect on the hydrogen-bond network and infrared spectrum of water was analyzed for different CNT diameters. The results provide new insights into the hydrogen bonding behavior of water confined in CNTs and offer a general platform for simulating such systems with quantum accuracy.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Saheli Mitra, Susana Marin-Aguilar, Srikanth Sastry, Frank Smallenburg, Giuseppe Foffi
Summary: This study investigates the correlation between local structure and propensity for structural rearrangement in glass forming liquids and glasses. The results show that in a cyclic shear deformation, particles with higher S-2 and lower n(tet) are more likely to undergo rearrangement, regardless of the average energies of the configurations and strain amplitude. Distinctive local ordering is observed outside the shear band region, with the formation of icosahedral clusters.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Correction
Chemistry, Physical
Frank Smallenburg
EUROPEAN PHYSICAL JOURNAL E
(2022)
Article
Chemistry, Physical
Rinske M. Alkemade, Emanuele Boattini, Laura Filion, Frank Smallenburg
Summary: In this study, three different machine learning algorithms were used to predict the dynamic properties of glassy materials. The results show that all three methods achieve similar accuracy when advanced structural descriptors are used. However, linear regression is significantly faster to train compared to the other methods.
JOURNAL OF CHEMICAL PHYSICS
(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
Physics, Multidisciplinary
Andreas Neophytou, Dwaipayan Chakrabarti, Francesco Sciortino
Summary: This article demonstrates through experiments that the liquid-liquid phase transition in tetrahedral networks can be described as a transition between an unentangled, low-density liquid and an entangled, high-density liquid, with a clear topological distinction between the two phases.
Article
Physics, Multidisciplinary
Lorenzo Rovigatti, Francesco Sciortino
Summary: Single-chain nanoparticles are polymeric objects with special structures, and the phase transition can be controlled by designing the arrangement of reactive monomers. The study of this structure is of great significance for controlling polymer bonding.
PHYSICAL REVIEW LETTERS
(2022)
Article
Chemistry, Physical
E. Lattuada, T. Pietrangeli, F. Sciortino
Summary: In this experiment, we investigated the equilibrium gel formation in a binary mixture of DNA nanostars. We found that two interpenetrating unconnected gels formed in the sample on cooling, with each gel forming at a temperature controlled by the selected binding DNA sequence. The dynamic light scattering correlation functions showed a non-common three-step relaxation process.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Riccardo Foffi, Francesco Sciortino
Summary: Multiple numerical studies have confirmed the existence of a liquid-liquid critical point and proposed various structural indicators to describe the associated phase transition. Analyzing simulations of near-critical supercooled water, it is found that most indicators are strongly correlated to density, suggesting a tight coupling between apparently distinct structural degrees of freedom near the critical point.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Physical
Camilla Beneduce, Diogo E. P. Pinto, Petr Sulc, Francesco Sciortino, John Russo
Summary: This study investigates the nucleation process of a binary mixture of patchy particles designed to nucleate into a diamond lattice. By combining Gibbs-ensemble simulations and direct nucleation simulations, the role of the liquid-gas metastable phase diagram on the nucleation process is revealed. The strongest enhancement of crystallization is found to occur at an azeotropic point with the same stoichiometric composition of the crystal.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Editorial Material
Chemistry, Physical
Michele Ceriotti, Lasse Jensen, David E. Manolopoulos, Todd Martinez, David R. Reichman, Francesco Sciortino, C. David Sherrill, Qiang Shi, Carlos Vega, Lai-Sheng Wang, Emily A. Weiss, Xiaoyang Zhu, Jenny Stein, Tianquan Lian
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Rinske M. Alkemade, Frank Smallenburg, Laura Filion
Summary: This study explores whether a simple linear regression algorithm combined with intelligently chosen structural order parameters can achieve the accuracy of the current advanced machine learning approaches for predicting dynamic propensity. The research finds that the structure of the cage state is highly predictive of the long-time dynamics of the system compared to the initial and inherent states. By combining the cage state information with the initial state, dynamic propensities can be predicted with unprecedented accuracy over a broad range of time scales, including the caging regime.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Francesco Guidarelli Mattioli, Francesco Sciortino, John Russo
Summary: We propose a new neural network potential that incorporates atomic fingerprints based on both two- and three-body contributions. These fingerprints probe distances and local orientational order. The training process of the proposed potential is simplified by using a small set of tunable parameters for the fingerprints. This approach improves the overall accuracy of the network representation and successfully reproduces the behavior of the mW model of water.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Francesco Guidarelli Mattioli, Francesco Sciortino, John Russo
Summary: Neural network potentials (NNPs) are increasingly used to study long time scale processes, such as crystal nucleation. It is unclear whether NN potentials trained on equilibrium liquid states can accurately describe nucleation processes. In this study, a NNP trained on a classical three-body potential for water accurately reproduces nucleation rates and free energy barriers, supporting the use of NNPs for studying nucleation events.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Multidisciplinary Sciences
Diogo E. P. Pinto, Petr Sulc, Francesco Sciortino, John Russo
Summary: The control over self-assembly of complex structures, particularly at the colloidal scale, has been a significant challenge in material science. The formation of amorphous aggregates often disrupts the desired assembly pathway. In this study, we investigate the self-assembly problem of three Archimedean shells using patchy particles as model building blocks. By recasting the assembly problem as a Boolean satisfiability problem, we find effective designs and selectively suppress unwanted structures.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Chemistry, Physical
Etienne Fayen, Marianne Imperor-Clerc, Laura Filion, Giuseppe Foffi, Frank Smallenburg
Summary: Hard spheres are a fundamental model system in soft matter physics and have been crucial in understanding classical condensed matter. Simulations show that a simple model system of two sizes of hard spheres can self-assemble into two distinct random-tiling quasicrystal phases. The formation of these quasicrystals demonstrates that entropy and geometrically compatible, densely packed tiles are sufficient for the self-assembly of colloidal quasicrystals.
