According to the mosaic scenario, relaxation in supercooled liquids is ruled by two competing mechanisms: surface tension, opposing the creation of local excitations, and entropy, providing the drive to the configurational rearrangement of a given region. We test this scenario through numerical simulations well below the Mode Coupling temperature. For an equilibrated configuration, we freeze all the particles outside a sphere and study the thermodynamics of this sphere. The frozen environment acts as a pinning field. Measuring the overlap between the unpinned and pinned equilibrium configurations of the sphere, we can see whether it has switched to a different state. We do not find any clear evidence of the mosaic scenario. Rather, our results seem compatible with the existence of a single (liquid) state. However, we find evidence of a growing static correlation length, apparently unrelated to the mosaic one.
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http://dx.doi.org/10.1103/PhysRevLett.98.187801 | DOI Listing |
Adv Mater
December 2024
Extreme Materials Research Center, Korea Institute of Science and Technology, 5, Hwarang-ro 14-gil, Seoul, Seongbuk-gu, 02792, Republic of Korea.
Additive manufacturing has sought active and interactive means of creating predictable structures with diverse materials. Compared to such active manufacturing tools, current crystallization strategies remain in statistical and passive programs of crystals via macroscale thermodynamic controllers, commonly lacking active means to intervene in crystal growth in a spatiotemporal manner. Herein, a strategy toward active and interactive programming and reprogramming of crystals, realized by real-time tangible feedback on growing crystals by delicately controlling the degree of in-situ, localized photopolymerization of polymeric structures via additive manufacturing is presented.
View Article and Find Full Text PDFJ Phys Chem B
December 2024
CAS Key Laboratory of Magnetic Materials and Devices, and Zhejiang Province Key Laboratory of Magnetic Materials and Application Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, China.
The glacial phase can be formed from supercooled liquid (SCL) in certain systems, which is called liquid-liquid transition (LLT). Revealing the nature of the glacial phase especially in a single-component system is crucial for understanding the LLT process. Here, by using flash differential scanning calorimetry and cold-field transmission electron microscopy, the structure of the d-mannitol glacial phase and the phase transition kinetics between the glacial phase and SCL were studied.
View Article and Find Full Text PDFPhys Rev E
November 2024
INQUISUR, Departamento de Química, Universidad Nacional del Sur (UNS)-CONICET, Avenida Alem 1253, 8000 Bahía Blanca, Argentina.
In this work, we shall study the role of threefold and fivefold coordination defects in the structure and dynamics of the hydrogen bond network of liquid water, with special emphasis on the glassy regime. A significant defect clusterization propensity will be made evident, with a prevalence of mixed pairs, that is, threefold- and fivefold-coordinated defects being first neighbors of each other. This structural analysis will enable us to determine the existence of defective and nondefective regions compatible with the high local density and low local density molecular states of liquid water, respectively.
View Article and Find Full Text PDFJ Phys Condens Matter
December 2024
Department of Materials, Imperial College London, Exhibition Road, London SW7 2AZ, United Kingdom.
While the glass transition is easy to identify macroscopically, the underlying atomic mechanisms which facilitate the transition from amorphous solid to fluid are still poorly understood. We conduct classical molecular dynamics simulations on a variety of inorganic glasses in order to identify these mechanisms. While also modelling larger systems, we find that the essential qualities which constitute a glass and its transition to a liquid are present even in systems containing only a few hundred atoms.
View Article and Find Full Text PDFJ Chem Phys
December 2024
Department of Chemistry, University of Wisconsin-Madison, 1101 University Ave., Madison, Wisconsin 53706, USA.
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