Article
Physics, Multidisciplinary
Gerhard Jung, Giulio Biroli, Ludovic Berthier
Summary: We propose GlassMLP, a machine learning framework that utilizes physics-inspired structural input to predict long-time dynamics in deeply supercooled liquids. Our deep neural network shows superior performance compared to existing methods, requiring less training data and fitting parameters. GlassMLP accurately predicts four-point dynamic correlations and the geometry of dynamic heterogeneity. The transferability across system sizes enables efficient study of temperature-dependent spatial dynamic correlations, revealing significant changes in the geometry of rearranging regions.
PHYSICAL REVIEW LETTERS
(2023)
Review
Chemistry, Multidisciplinary
Indrajit Tah, Anoop Mutneja, Smarajit Karmakar
Summary: Glasses are prevalent in nature and play a significant role in our daily lives. The dynamics of glass-forming systems, ranging from microscopic to macroscopic scales, exhibit slow and heterogeneous behaviors. Recent research has shown that there are growing dynamic and static correlation lengths associated with the observed dynamical heterogeneity and rapid rise in viscosity, highlighting the complexity of glassy dynamics.
Article
Biochemistry & Molecular Biology
Giuseppe Porpora, Francesco Rusciano, Raffaele Pastore, Francesco Greco
Summary: Glass transition is an intriguing open issue in molecular liquids, and recent research has found that the relationship between macroscopic timescales and cage-jump quantities changes on approaching the glass transition.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Chemistry, Physical
W. Zhu, Y. Xia, B. G. Aitken, S. Sen
Summary: In deeply supercooled regime, the onset of shear thinning and transition from Newtonian to non-Newtonian behavior in select chalcogenide and oxide network glass-forming liquids were studied, showing a temperature-dependent relationship. The shear thinning mechanism in network liquids appears to be fundamentally different from other types of glass-forming liquids, with reduced shear rate decreasing with increasing temperature, particularly with higher fragility.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Materials Science, Ceramics
Pierre Lucas
Summary: Fragile-to-strong (FTS) transitions have been observed in all categories of glass-forming systems, leading to a change from Arrhenius to non-Arrhenius viscosity behavior, along with anomalies in various thermodynamic variables. Experimental evidence supports the presence of FTS transitions, where a peak in heat capacity and density extrema with a negative expansion coefficient are found. Spectroscopic analyses also reveal distinct structural changes across these liquid-liquid transitions. Reports of FTS transitions in each category of liquid are reviewed.
JOURNAL OF NON-CRYSTALLINE SOLIDS
(2021)
Article
Multidisciplinary Sciences
Matthew A. Harris, Thomas Kinsey, Durgesh Wagle, Gary A. Baker, Joshua Sangoro
Summary: A liquid-liquid transition (LLT) is a transformation from one liquid to another through a first-order transition, fundamental to understanding the liquid state. While LLT has been reported in some materials, experimental evidence for its existence in many molecular liquids remains controversial. Studying the local order and structural dynamics across an LLT provides unprecedented possibilities for understanding the nature of the liquid state.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Review
Physics, Multidisciplinary
Vladimir N. Novikov, Alexei P. Sokolov
Summary: This review focuses on the mechanisms that control the steepness of the temperature dependence of structural relaxation in glass-forming liquids. It discusses the specific case of polymeric glass-forming liquids and the possible role of quantum effects in the glass transition.
Article
Chemistry, Physical
Austin D. Hartley, William F. Drayer, Asieh Ghanekarade, David S. Simmons
Summary: Glass-forming liquids exhibit dynamic heterogeneity at both the surface and bulk, but with different characteristics and spatial correlations. The study also suggests that slow dynamic gradients near interfaces extend further into the film than fast dynamic gradients.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
B. Yao, Z. Wojnarowska, M. Paluch
Summary: The ultimate aim of researchers is to predict the properties of matter based on molecular structure, but achieving this goal is still challenging. By comparing two compounds, benzene and cyclohexane, which differ only in the type of six-carbon ring, the study demonstrates how aromaticity affects the relaxation dynamics behavior of supercooled liquid and glass. Through experiments under ambient and elevated pressure, the researchers identified which dynamic and thermodynamic quantities are sensitive to such structural differences and which are not.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Materials Science, Ceramics
A. A. Lukichev
Summary: This paper proposes new simple power functions to describe the relationship between the viscosity of glass-forming substances and temperature and pressure. These functions are based on an activation model theory and are shown to be in good agreement with practical dependencies. The new functions serve as a simple and effective tool for investigating the properties of glass-formers, revealing unknown effects and variable fragility.
JOURNAL OF NON-CRYSTALLINE SOLIDS
(2021)
Article
Chemistry, Physical
Nele N. Striker, Irina Lokteva, Michael Dartsch, Francesco Dallari, Claudia Goy, Fabian Westermeier, Verena Markmann, Svenja C. Hovelmann, Gerhard Grubel, Felix Lehmkuhler
Summary: The dynamics and time scales of higher-order correlations in supercooled colloidal systems were studied using X-ray photon correlation spectroscopy (XPCS) and X-ray cross-correlation analysis (XCCA). The results showed the typical slowing of the dynamics of a hard sphere system when approaching the glass transition. The time scales of higher-order correlations were probed using a novel time correlation function g(C), revealing that the local orders within the sample become more long-lived for larger volume fractions.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Mengtan Liu, Ryan D. McGillicuddy, Hung Vuong, Songsheng Tao, Adam H. Slavney, Miguel Gonzalez, Simon J. L. Billinge, Jarad A. Mason
Summary: Molten phases of metal-organic networks offer exciting opportunities for using coordination chemistry principles to access liquids and glasses with unique and tunable structures and properties. General thermodynamic strategies provide increased enthalpic and entropic driving force for reversible, low-temperature melting transitions in extended coordination solids, illustrated through a systematic study of bis(acetamide)-based networks with record-low melting temperatures. Weak coordination bonds, conformationally flexible bridging ligands, and weak electrostatic interactions contribute to the low melting temperatures of these compounds, reducing enthalpy and increasing entropy of fusion.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Thomas McKenzie-Smith, Jack F. Douglas, Francis W. Starr
Summary: This study explores the temperature dependence of the structural relaxation time in glass-forming materials and aims to find a unified description. Both the string model and the localization model are examined and found to describe the relaxation behavior well. By comparing the model parameters, a connection between the local caging scale and the entropy of activation for molecular rearrangements in the string model is established.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Nanoscience & Nanotechnology
Nannan Ren, Lina Hu, Bing Wang, Kaikai Song, Pengfei Guan
Summary: This study investigates the evolution of hidden structural topological features associated with the non-Arrhenius crossover in metallic glass-forming liquids through molecular dynamics simulations and topological order analysis. It reveals that the cooperative motions of atoms with k > 3 developing a stable topological network contribute to the non-Arrhenius behavior below the crossover temperature T-A, shedding light on the structural origin of relaxation dynamics in metallic glass-forming liquids.
SCRIPTA MATERIALIA
(2021)
Article
Materials Science, Ceramics
Y. X. Chen, S. P. Pan, X. Q. Lu, H. Kang, Y. H. Zhang, M. Zhang, S. D. Feng, K. L. Ngai, L. M. Wang
Summary: The study reveals the existence of unusual caged dynamics in metallic glass-forming liquids with strong atomic interactions. The mechanism of caged dynamics is found to be related to chemical order, Voronoi polyhedra, and covalent-like bonds.
JOURNAL OF NON-CRYSTALLINE SOLIDS
(2022)
