Article
Chemistry, Physical
Dean Eaton, Ivan Saika-Voivod, Richard K. Bowles, Peter H. Poole
Summary: The authors tested the theoretical free energy surface (FES) for two-step nucleation (TSN) by comparing it to numerical results from Monte Carlo simulations, finding that the theory successfully predicted FES over a range of thermodynamic conditions. This demonstrates that Iwamatsu's extension of classical nucleation theory provides an excellent framework for understanding the thermodynamics of TSN.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Physics, Condensed Matter
Hao Lu, Quanming Xu, Jianyang Wu, Rongdun Hong, Zhisen Zhang
Summary: In this study, molecular dynamics simulations were used to investigate the ice nucleation on a rigid surface model with different surface dipole strength and orientation. The results indicate that the molecular orientations of interfacial component play a critical role in promoting ice nucleation, highlighting the significance beyond traditional lattice match and length similarity between substrate and new-formed crystal.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2021)
Article
Chemistry, Physical
Ruel Cedeno, Romain Grossier, Nadine Candoni, Nicolas Levernier, Adrian Flood, Stephane Veesler
Summary: In this study, we present the first stochastic treatment of NaCl-water nucleation kinetics using a recently developed microfluidic system and evaporation model. Our experimental results show an excellent agreement between the measured interfacial energies, extracted from a modified Poisson distribution of nucleation time, and theoretical predictions. Additionally, our analysis of nucleation parameters in microdroplets of different sizes reveals an interesting interplay between kinetic confinement and shifting of nucleation mechanisms. Overall, our findings emphasize the importance of treating nucleation stochastically rather than deterministically to bridge the gap between theory and experiment.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
M. Asim Sajid Al-Hanafi, Mhd Bashir Alsirawan, Colin C. Seaton, Thomas Swift, Sudhir Pagire, Venu R. Vangala, Adrian L. Kelly, Anant Paradkar
Summary: Cocrystals, formed by the bonding of two molecules in a single crystal lattice, have wide applications in improving the solubility of poorly soluble pharmaceuticals. The study shows that the cocrystallization reaction can prevent the formation of unwanted oily phase during liquid-liquid phase separation.
CRYSTAL GROWTH & DESIGN
(2022)
Article
Multidisciplinary Sciences
Michael Benedict Davies, Martin Fitzner, Angelos Michaelides
Summary: Through molecular dynamics simulations, researchers have found that many different substrates can promote the formation of pristine I-c, I-c can be selectively nucleated even with mild supercooling, the water contact layer's resemblance to a face of ice is the key factor determining the polytype selectivity and nucleation temperature, and substrate lattice match to ice is not indicative of the polytype obtained.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Xing He, Ding-Shyue Yang
Summary: A clear understanding of solid-molecule interfacial structures is crucial for comprehending interfacial phenomena and the interplay of surface effects and intermolecular forces. The study on the structures and phase-transition behavior of ethanol assemblies deposited on highly orientated pyrolytic graphite revealed a complex multistep process, reflecting a delicate balance between interfacial and intermolecular forces, and molecular free energy.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Multidisciplinary Sciences
Mark A. Holden, James M. Campbell, Fiona C. Meldrum, Benjamin J. Murray, Hugo K. Christenson
Summary: The nucleation of ice crystals in clouds is influenced by different meteorological conditions, leading to distinct pathways of immersion freezing and deposition nucleation. Experimental results on two atmospheric minerals show little correlation between active sites in these two modes, suggesting different properties determine the activity of nucleation sites for each mode. Therefore, the ability to nucleate is pathway dependent, and mode of nucleation must be considered when applying experimental data in cloud models.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Ignacio Sanchez-Burgos, Eduardo Sanz, Carlos Vega, Jorge R. Espinosa
Summary: The computational characterization of polymorphic nucleation competition between face-centered cubic (fcc) and hexagonal-close packed (hcp) hard-sphere crystal phases was conducted, revealing that the hcp phase may have a slightly higher interfacial free energy than the fcc phase, leading to a decreased propensity to nucleate from the liquid. The abundance of each polymorph in grown crystals from different types of nuclei and the maintenance of polymorphic structure in post-critical crystals were also analyzed, providing insights into the intricate puzzle of colloidal hard-sphere crystallization.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Xiangyue Meng, Yunfei Li, Yizhi Qu, Haining Chen, Nan Jiang, Minghua Li, Ding-Jiang Xue, Jin-Song Hu, Hui Huang, Shihe Yang
Summary: The crystallization kinetics of tin halide perovskites were modulated through a non-classical nucleation mechanism, leading to improved efficiency and stability of lead-free perovskite solar cells.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Mithun Ghosh, Ding-Shyue Yang
Summary: The study reveals that a hydrophobic self-assembled monolayer (SAM) surface can influence the crystallization of acetonitrile, ethanol, and methanol despite the absence of significant substrate-molecule forces. Acetonitrile and ethanol show sustaining vertical assembly order with long-range crystalline structures, while methanol exhibits thickness-dependent ordering with changes in epitaxy and strain.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Multidisciplinary Sciences
Xiangwen Liu, See Wee Chee, Sanoj Raj, Michal Sawczyk, Petr Kral, Utkur Mirsaidov
Summary: Metal-organic frameworks (MOFs) are crystalline nanoporous materials with great industrial application potential. Understanding the nucleation and growth stages from a solution is crucial for design and synthesis. The study reveals a three-step pathway for MOF nucleation via liquid-liquid phase separation, direct condensation into an amorphous aggregate, and crystallization into MOF, providing evidence for nonclassical nucleation pathways.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Fausto Martelli, Jeremy C. Palmer
Summary: We investigated the spontaneous crystallization of water in the ST2 model under deeply supercooled conditions using molecular dynamics simulations. The ST2 model separates into low-density liquid and high-density liquid phases, promoting the formation of a sub-critical ice nucleus. Polymorphic selection favors the formation of cubic ice over hexagonal ice, and the critical nucleus absorbs both types of crystallites in the liquid phase.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Multidisciplinary Sciences
Xabier M. Aretxabaleta, Jon Lopez-Zorrilla, Inigo Etxebarria, Hegoi Manzano
Summary: The authors of this study used atomistic simulations to investigate the nucleation process of C-S-H in cement hydration. They proposed a possible formation pathway and identified a potential C-S-H basic building block.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Adam McElligott, Andre Guerra, Alexia Denoncourt, Alejandro D. Rey, Phillip Servio
Summary: This study investigates the freezing of up to three simultaneous THF hydrate droplets using acoustic levitation, revealing different nucleation mechanisms and structural inhomogeneities within the droplets.
Review
Chemistry, Multidisciplinary
Leah Fuhrman Javitt, Sofia Curland, Isabelle Weissbuch, David Ehre, Meir Lahav, Igor Lubomirsky
Summary: The ability to control the icing temperature of supercooled water (SCW) is of supreme importance in subfields of pure and applied sciences. In this Account, it is demonstrated that heterogeneous electrofreezing of SCW is a chemical process influenced by an electric field and specific ions, by capitalizing on the properties of polar crystals.
ACCOUNTS OF CHEMICAL RESEARCH
(2022)