Surface Induced Crystallization in Supercooled Tetrahedral Liquids

Abstract

Freezing is a fundamental physical phenomenon that has been studied over many decades; yet the role played by surfaces in determining nucleation has remained elusive. Here we report direct computational evidence of surface induced nucleation in supercooled systems with a negative slope of their melting line (dP/dT < 0). This unexpected result is related to the density decrease occurring upon crystallization, and to surface tension facilitating the initial nucleus formation. Our findings support the hypothesis of surface induced crystallization of ice in the atmosphere, and provide insight, at the atomistic level, into nucleation mechanisms of widely used semiconductors.

5 pages, 4 figures

References in corpus (5)

• Simulating rare events in equilibrium or non-equilibrium stochastic systems
• Forward Flux Sampling-type schemes for simulating rare events: Efficiency analysis
• Surface Crystallization in a Liquid AuSi Alloy
• Tuning of tetrahedrality in a silicon potential yields a series of monatomic (metal-like) glassformers of very high fragility
• Local structure of liquid carbon controls diamond nucleation

Cited by in corpus (22)

• Crystal Nucleation in Liquids: Open Questions and Future Challenges in Molecular Dynamics Simulations
• Homogeneous ice nucleation at moderate supercooling from molecular simulation
• Direct Calculation of Ice Homogeneous Nucleation Rate for a Molecular Model of Water
• Thermodynamically Driven Assemblies and Liquid-liquid Phase Separations in Biology
• Studying Rare Events using Forward-Flux Sampling: Recent Breakthroughs and Future Outlook
• Suppression of Sub-surface Freezing in Free-Standing Thin Films of a Coarse-grained Model of Water
• Spontaneous Imbibition Dynamics of an n-Alkane in Nanopores: Evidence of Meniscus Freezing and Monolayer Sticking
• Nucleation at the contact line observed on nano-textured surfaces
• Forward Flux Sampling Calculation of Homogeneous Nucleation Rates from Aqueous NaCl Solutions
• Forward-Flux Sampling with Jumpy Order Parameters
• Nucleation barriers in tetrahedral liquids spanning glassy and crystallizing regimes
• Induced Charge Anisotropy: a Hidden Variable Affecting Ion Transport through Membranes
• Computational investigation of structure, dynamics and nucleation kinetics of a family of modified Stillinger-Weber model fluids in bulk and free-standing thin films
• Role of Nanoscale Interfacial Proximity in Contact Freezing in Water
• Perspective: Surface Freezing in Water: A Nexus of Experiments and Simulations
• Inhomogeneous Relaxation Dynamics and Phase Behaviour of a Liquid Crystal Confined in a Nanoporous Solid
• Can xenon in water inhibit ice growth? Molecular dynamics of phase transitions in water$-$Xe system
• Thermotropic interface and core relaxation dynamics of liquid crystals in silica glass nanochannels: A dielectric spectroscopy study
• Nucleation and droplet growth from supersaturated vapor at temperatures below the triple point temperature
• Ideal Conductor Model: An analytical finite-size correction for non-equilibrium molecular dynamics simulations of ion transport through nanoporous membranes
• Chemical Ordering and Crystal Nucleation at the Liquid Surface: A Comparison of ${\mathrm{Cu}}_{50}{\mathrm{Zr}}_{50}$ and ${\mathrm{Ni}}_{50}{\mathrm{Al}}_{50}$ Alloys
• The Impact of Hydration Shell Inclusion and Chain Exclusion in the Efficacy of Reaction Coordinates for Homogeneous and Heterogeneous Ice Nucleation