Related papers: Non-classical pathways of crystallization in collo…
The interplay between densification and positional ordering during the process of crystal nucleation is a greatly investigated topic. Even for the simplest colloidal model -- hard spheres -- there has been much debate regarding the…
Modulating liquid-to-solid transitions and the resulting crystalline structure for tailored properties is much desired. Colloidal systems are exemplary to this end, but the fundamental knowledge gaps in relating the influence of…
Viscoelastic phase separation of colloidal suspensions can be interrupted to form gels either by glass transition or by crystallization. With a new confocal microscopy protocol, we follow the entire kinetics of phase separation, from…
Studies of nucleation generally focus on the properties of the critical cluster, but the presence of defects within the crystal lattice means that the population of nuclei necessarily evolve through a distribution of pre-critical clusters…
This thesis can be divided into two independent parts. In the first part of this thesis, we focus on studying the kinetic pathways of nucleation in colloidal systems. In Chapter 2, we briefly introduce the relevant theory of nucleation,…
Understanding the underlying mechanism of crystal nucleation during solidification is a fundamental aspect in the prediction and control of materials properties. Classical nucleation theory (CNT) assumes that homogeneous nucleation occurs…
Crystal growth and crystal coalescence processes in supercooled systems strongly depend on the concentration of crystallization centers. We perform atomistic dynamics simulations of the crystallization process in the ultrathin metallic film…
The emergence upon cooling of an ordered solid phase from a liquid is a remarkable example of self-assembly, which has also major practical relevance. Here, we use a recently developed committor-based enhanced sampling method [Kang et al.,…
Over recent years, molecular simulations have provided invaluable insights into the microscopic processes governing the initial stages of crystal nucleation and growth. A key aspect that has been observed in many different systems is the…
Using state-of-the-art rare-event sampling simulations, we precisely characterize the nucleation of liquid droplets from a supersaturated Lennard-Jones gas and uncover a key physical feature: critical clusters nucleate with a density that…
Freezing of charged colloids on square or triangular two-dimensional periodic substrates has been recently shown to realize a rich variety of orientational orders. We propose a theoretical framework to analyze the corresponding structures.…
NaCl crystal nucleation from metastable solutions has long been considered to occur according to a single-step mechanism. Recent experimental observations suggest that NaCl crystals emerge from disordered intermediates which is seemingly at…
We attempt a classification of different colloidal gels based on colloid-colloid interactions. We discriminate primarily between non-equilibrium and equilibrium routes to gelation, the former case being slaved to thermodynamic phase…
Bifurcations in kinetic pathways decide the evolution of a system. An example is crystallization, in which the thermodynamically stable polymorph may not form due to kinetic hindrance. Here, we use confined self-assembly to investigate the…
Micrometre sized colloidal particles can be viewed as large atoms with tailorable size, shape and interactions. These building blocks can assemble into extremely rich structures and phases, in which the thermal motions of particles can be…
Despite numerous efforts from numerical approaches to complement experimental measurements, several fundamental challenges have still hindered one's ability to truly provide an atomistic picture of the nucleation process in nanocrystals.…
The kinetic mechanisms underlying bottom-up assembly of colloidal particles have been widely investigated in efforts to control crystallization pathways and to direct growth into targeted superstructures for applications including photonic…
We study the conditions under which and how an imposed cluster of fixed colloidal particles at prescribed positions triggers crystal nucleation from a metastable colloidal fluid. Dynamical density functional theory of freezing and Brownian…
The interplay between crystal nucleation and the structure of the metastable fluid has been a topic of significant debate over recent years. In particular, it has been suggested that even in simple model systems such as hard or charged…
According to classical nucleation theory, a crystal grows from a small nucleus that already bears the symmetry of its end phase - but experiments with colloids now reveal that, from an amorphous precursor, crystallites with different…