Article
Physics, Multidisciplinary
Xiaoyan Sun, Huaguang Wang, Hao Feng, Zexin Zhang, Yuqiang Ma
Summary: Identification of the glass formation process under various conditions is crucial for understanding glass transitions and developing glass materials. By studying colloidal suspensions of monodisperse microspheres, researchers found that pinning a fraction of microspheres can drive the transition from crystal to glass. The dynamics show a non-monotonic change with increasing pinning fraction, highlighting the competition between disorder enhancing the dynamics and pinning hindering the particle motions.
CHINESE PHYSICS LETTERS
(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
Physics, Fluids & Plasmas
Jiankai Hu, Luhui Ning, Rui Liu, Mingcheng Yang, Ke Chen
Summary: By using video microscopy, the long-time diffusion coefficients of colloidal particles at different concentrations were measured. It was found that the measured values deviate from theoretical predictions in the supercooled regime. However, the theoretical diffusion relation can be recovered by assigning an effective mass proportional to the size of structurally correlated clusters to the diffusing particles, which provides an indirect method to probe the growth of static correlation length scales approaching the glass transition. This method was validated in quasi-two-dimensional experiments of crystallization of mono-disperse colloids.
Article
Multidisciplinary Sciences
T. J. Bullard, M. A. Susner, K. M. Taddei, J. A. Brant, T. J. Haugan
Summary: The study investigates the magnetic and structural properties of the solid solution CuAl2(1-x)Ga2xO4, demonstrating a shift in Cu2+ ions from tetrahedral to octahedral sites with increasing Ga3+ ion concentration. While most of the solution exhibits glassy behavior, the trend is towards decreasing magnetic frustration as the Cu2+ ion moves to the B-site, with exceptions in the x = 0.1 and 0.2 members which show delayed spin glass transition. These members are suggested as additional candidates for investigating highly frustrated exotic quantum states.
SCIENTIFIC REPORTS
(2021)
Article
Physics, Multidisciplinary
Yiming Xia, Xiunan Yang, Junchao Huang, Rui Liu, Ning Xu, Mingcheng Yang, Ke Chen
Summary: We constructed structural order parameters based on local angular and radial distribution functions in dense colloidal suspensions and found significant correlations between these parameters and local dynamics. In particular, the correlation between local orientational order and dynamical heterogeneity was consistently higher than the correlation between conventional two-body structural entropy and local dynamics. The structure-dynamics correlations can be explained by an excitation model where the energy barrier depends on local structural order. Our results suggest that in dense disordered packings, local orientational order is higher than translational order and plays a more important role in determining the dynamics in glassy systems.
PHYSICAL REVIEW LETTERS
(2023)
Article
Materials Science, Ceramics
M. Micoulaut, H. Flores-Ruiz
Summary: The optoelectronic properties of prototypal Telluride amorphous phase-change materials (GeTe and Ge2Sb2Te5) are investigated through ab initio molecular dynamics simulations. It is found that the local tetrahedral germanium geometries significantly influence the targeted properties, with lower momenta and dual localization characteristics.
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
(2023)
Article
Physics, Fluids & Plasmas
Peter Olsson
Summary: In this study, extensive simulations are conducted to investigate the velocity distribution in a two-dimensional shear-driven jamming model. Two distinct processes, the slow process and the fast process, are found to contribute to the velocity distribution and shear viscosity. It is also observed that the slow process dominates the collective particle motion.
Article
Materials Science, Ceramics
Jiri Malek
Summary: The structural relaxation of chalcogenide glasses is discussed using the TNM formalism, and the TNM parameters of different glass compositions are compared. It is shown that the R-f(10) estimated at 10 K below T-g can be used to predict the structural relaxation kinetics of various amorphous materials. Chalcogenide glasses are compared to oxide glasses and organic polymers, and a well-defined pattern is observed in the R-f(10) versus sigma plot.
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
(2023)
Article
Physics, Fluids & Plasmas
U. Buchenau
Summary: The shear misfit model is used to study highly viscous flow and predicts the terminal stage of the flow. It also provides insight into density fluctuations and the relationship between adiabatic and isothermal compressibility jumps at the glass transition.
Article
Physics, Multidisciplinary
Yanshuang Chen, Zefang Ye, Kexin Wang, Jiping Huang, Hua Tong, Yuliang Jin, Ke Chen, Hajime Tanaka, Peng Tan
Summary: Glasses can relax internally even when their structure is frozen. In a two-dimensional glass former, non-constrained bonds survive the freezing of structural relaxation, leading to persistent internal relaxation. This study directly visualizes the internal relaxations in a glass through observations of a mechanically driven granular system, revealing the emergence of slow beta relaxation as the structure relaxation freezes.
Article
Chemistry, Physical
Gang Sun, Peter Harrowell
Summary: This paper proposes a method to develop a general atomic level description of amorphous solidification by measuring a measure of atomic restraint. By defining the measure using instantaneous normal modes, the differences between fragile and strong liquids and the collective length scale of the supercooled liquid can be taken into account.
JOURNAL OF CHEMICAL PHYSICS
(2022)
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
Crystallography
Aleksandra Deptuch, Malgorzata Jasiurkowska-Delaporte, Ewa Juszynska-Galazka, Anna Drzewicz, Magdalena Urbanska
Summary: The vitrification and cold crystallization of the antiferroelectric hexatic smectic X-A* phase for (S)-4 '-(1-methylheptylcarbonyl)biphenyl-4-yl 4-[5-(2,2,3,3,4,4,4-heptafluorobutoxy) heptyl-1-oxy]benzoate are investigated. It is found that the kinetics of both isothermal cold crystallization and melt crystallization are mainly controlled by diffusion, with an activation energy of 114 kJ/mol. A weak relaxation process is observed in the crystal phase, implying the presence of a conformationally disordered crystal phase. The fragility parameter of the glass former is estimated to be 94.5, indicating a relatively high fragility.
Article
Materials Science, Ceramics
Lorena R. Rodrigues, Alexander S. Abyzov, Vladimir M. Fokin, Edgar Dutra Zanotto
Summary: This article discusses the influence of structural relaxation on crystal nucleation process. It shows that structural relaxation has a significant impact on nucleation rate at low temperatures, leading to a continuous increase before reaching a steady state. The study also explains the alleged breakdown of CNT at low temperatures and reveals a significantly lower actual maximum nucleation temperature than previously reported values.
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
(2021)
Article
Chemistry, Physical
Ranko Richert, Jan P. Gabriel, Erik Thoms
Summary: This study compares structural relaxation and structural recovery dynamics for molecular glass-formers measured by dielectric techniques, finding that structural recovery restores ergodicity while structural relaxation characterizes fluctuations in the system at equilibrium. The research shows that structural recovery is linked to rate exchange and is distinct from structural relaxation dynamics, even in the limit of small perturbations. This contrasts the standard assumption in physical aging models, which assume the identical responses of both in small perturbation limits.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Materials Science, Multidisciplinary
Bradley Duncan, Robert D. Weeks, Benjamin Barclay, Devon Beck, Patrick Bluem, Roberto Rojas, Maxwell Plaut, John Russo, Sebastien G. M. Uzel, Jennifer A. Lewis, Theodore Fedynyshyn
Summary: In this study, low-loss graded dielectric materials were successfully designed and printed using active mixing of nanocomposite inks. This method enables the rapid fabrication of high-performance RF devices with locally tunable dielectric properties.
ADVANCED MATERIALS TECHNOLOGIES
(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)
Article
Chemistry, Physical
Fergus Moore, John Russo, Tanniemola B. B. Liverpool, C. Patrick Royall
Summary: In this study, the structural and dynamical properties of active Brownian particles (ABPs) in random environments are explored. It is found that confinement increases the heterogeneity of the dynamics, resulting in the appearance of new populations of absorbed and localized particles near the obstacles. This heterogeneity has a profound impact on the motility induced phase separation exhibited by the particles at high activity, ranging from nucleation and growth in random disorder to a complex phase separation in porous environments.
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
Chemistry, Physical
Zhenhao Yu, Rui Shi, Hajime Tanaka
Summary: Water exhibits anomalous thermodynamic and kinetic properties, such as a maximum density at 4 degrees C and a viscosity decrease under pressure. The presence of a second critical point has been attributed to these anomalies. Through extensive molecular dynamics simulations of the TIP4P/2005 water model, we find that a hierarchical two-state model based on cooperative formation of tetrahedral structures via hydrogen bonding can unify the description of the structure, thermodynamic, and kinetic anomalies and criticality of water. This suggests the possible existence of a second critical point in water.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Physics, Multidisciplinary
Hideyo Tsurusawa, Hajime Tanaka
Summary: Experiments reveal a hierarchical structural ordering driven by local potential energy in amorphous gels, making them distinct from amorphous glasses. This ordering is driven by the potential energy, not free energy. These findings will deepen our understanding of gel and glass.
Article
Physics, Multidisciplinary
Yanshuang Chen, Zefang Ye, Kexin Wang, Jiping Huang, Hua Tong, Yuliang Jin, Ke Chen, Hajime Tanaka, Peng Tan
Summary: Glasses can relax internally even when their structure is frozen. In a two-dimensional glass former, non-constrained bonds survive the freezing of structural relaxation, leading to persistent internal relaxation. This study directly visualizes the internal relaxations in a glass through observations of a mechanically driven granular system, revealing the emergence of slow beta relaxation as the structure relaxation freezes.
Article
Physics, Multidisciplinary
Fabio Leoni, Fausto Martelli, C. Patrick Royall, John Russo
Summary: Glasses obtained from vapor deposition on a cold substrate have superior thermodynamic and kinetic stability compared to ordinary glasses due to the presence of locally favored structures (LFSs) that enhance stability near the free surface. Molecular dynamics simulations reveal that the occurrence of LFSs correlates with the stability of vapor deposited glasses, reaching a maximum at the optimal deposition temperature.
PHYSICAL REVIEW LETTERS
(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
Taiki Yanagishima, John Russo, Roel P. A. Dullens, Hajime Tanaka
Summary: Research shows that the preparation protocol of glass determines the crystal growth mode. Traditional glass, prepared by fast quenching, exhibits fast growth with active interface dynamics, while uniform glass, prepared by density homogenization, grows via intermittent avalanche-like dynamics localized at the interface, combining localized mechanical defects and exceptional mechanical stability imposed by the glass phase.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Multidisciplinary Sciences
Hua Tong, Hajime Tanaka
Summary: Understanding the structural ordering upon slow cooling in the absence of crystallization or phase separation is crucial for understanding glass transition. We found that the exotic compositional order has a direct impact on the structural relaxation dynamics, even without any thermodynamic signature. This raises fundamental questions about the role of unconventional structural ordering in glass transition.
NATURE COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Rui Shi, Anthony J. Cooper, Hajime Tanaka
Summary: The behaviour of ions solvated in water is highly ion-specific and can be explained by considering the interplay between ion-water and inter-water interactions as well as the bond-orientational order of the hydration shell. This study provides insight into the ion-specific effects observed in salt solutions and their impact on solution dynamics. The findings have fundamental implications for ionic processes in aqueous solutions, offering a physical principle for electrolyte design and application.
NATURE COMMUNICATIONS
(2023)
Article
Physics, Multidisciplinary
Yuan-Chao Hu, Hajime Tanaka
Summary: Nonphononic vibrations have been identified as a fundamental feature that differentiates glasses from crystals. By studying the vibrational properties of three-dimensional model glasses, it has been found that stringlike vibrations are the universal origin of the boson peak in both 2D and 3D glasses with isotropic interactions. Furthermore, these vibrations coincide with the Ioffe-Regel limit of transverse phonons. These findings shed light on the origin of low-temperature glass anomalies and inspire further research.
PHYSICAL REVIEW RESEARCH
(2023)
Article
Chemistry, Physical
Fabio Leoni, Hajime Tanaka, John Russo
Summary: This study numerically investigates the nucleation process during the deposition of a glassformer and compares it with quenched counterpart and bulk system. It is found that all three systems uniformly nucleate crystals within a certain temperature range. The deposited layer shows the formation of ordered domains, with faster relaxation dynamics towards the free surface even in its as-deposited state. Additionally, the nucleus initially grows in an isotropic symmetrical manner but eventually shows sub-3D growth with a preference for growth along the basal plane, regardless of the layer production procedure.
JOURNAL OF MOLECULAR LIQUIDS
(2023)