arXiv subjects

Sam Oaks-Leaf

Publications and source records attributed to Sam Oaks-Leaf.

5 recordsLinked to original sources

arXiv2026

Size-Dependent Growth Rates Amplify Infinitesimal Asymmetry in Nanocrystals

The kinetic Wulff construction predicts symmetric nonequilibrium shapes when crystallographically equivalent facets share a fixed growth rate. However, nanocrystals grow through finite facets whose nucleation barriers and ligand coverages depend on facet size. Here we develop a size-dependent kinetic construction and show that as a consequence infinitesimal seed asymmetries can be amplified into strongly asymmetric nanocrystal morphologies even when all symmetry-related facets obey the same microscopic growth law. Spatially heterogeneous nucleation rates and boundary limited growth generate facet growth velocities that depend on size, and deterministic shape evolution translates these local rates into global shape symmetry breaking. We illustrate the mechanism of persistent anisotropic growth on square and triangular lattices in two dimensions and on FCC seeds in three dimensions, where cuboctahedra can evolve toward rods or tetrahedra depending on which facet-area perturbations are amplified.

cond-mat.mtrl-sci↗

arXiv2026

Visualizing Millisecond Atomic Dynamics of Nanocrystals in Liquid

Atomic structures of nanomaterials are inherently dynamic, continuously reshaped through interactions with chemical species and external stimuli. Such dynamics are further amplified as the size and dimensionality of nanomaterials are reduced. Despite advances in analytical methods, it remains challenging to capture structural dynamics of nanomaterials in reactive environments with both atomic spatial resolution and commensurate temporal resolution. Here, we directly visualize atomic-scale dynamics of gold (Au) nanocrystals in reactive liquid environments with millisecond-speed liquid cell electron microscopy (EM) and deep-learning denoising. We uncover reversible fluctuations in local crystallinity of Au nanocrystals dependent on the surrounding chemical environment. These transient fluctuations, driven by interactions at nanocrystal-liquid interfaces, critically influence dissolution kinetics and grain boundary relaxation. By overcoming the spatiotemporal limitations in conventional liquid cell EM, our findings provide insights into how transient nanoscale structures dictate the stability and reactivity of nanomaterials.

cond-mat.mtrl-sci↗

arXiv2025

Nanocrystal Geometry Governs Phase Transformation Pathways in Palladium Hydride

Pathways and structural dynamics of phase transformations impact performance of materials in energy and information storage technologies. Palladium hydride ($\mathrm{PdH}_x$) nanocrystals are an ideal model system for studying solute-induced phase transformations, where elastic energy from lattice mismatch between $\alpha$-$\mathrm{PdH}_x$ and $\beta$-$\mathrm{PdH}_x$ phases is often considered a key to determining the transformation pathways. $\alpha/\beta$-$\mathrm{PdH}_x$ interfacial elastic energy is affected by the confined geometry of a nanocrystal. However, how nanocrystal geometry influences phase transformation pathways is largely unknown. Using in situ liquid phase transmission electron microscopy, we directly visualize hydrogenation in Pd nanocrystals with two geometries -- a nanocube and a hexagonal nanoplate. Both follow similar sequences of an initially curved nucleus, interface flattening, and reverse-stage nucleation; however, their evolving $\alpha/\beta$-$\mathrm{PdH}_x$ interfaces exhibit geometry-dependent crystallographic alignments. In nanocubes, $\{100\}$-aligned configurations conform to static elastic energy ordering, representing a pathway that maintains a local mechanical equilibrium, whereas nanoplates display both $\{110\}$- and $\{211\}$-aligned interfaces. Theoretical simulations show that geometry determines the accessibility of alternative phase transformation pathways as the system is driven far from equilibrium during hydrogenation. These findings identify geometry as a fundamental parameter for directing phase transformation pathways, offering design principles for accessing atypical configurations and improving properties of intercalation-based devices.

cond-mat.mes-hall↗

arXiv2025

Mechanism of Shape Symmetry Breaking in Surfactant Mediated Crystal Growth

We present a dynamical model of crystal growth, in which it is possible to reliably achieve asymmetric products, beginning from symmetric initial conditions and growing within an isotropic environment. The asymmetric growth is the result of a positive feedback mechanism that amplifies the effect of thermal fluctuations in the coverage of surfactants on the growing crystalline facets. Within our simple model, we are able to understand the kinetic and thermodynamic factors involved in both the onset of symmetry breaking and the persistence of anisotropic growth. We demonstrate that the mechanism is general by studying models with increasing complexity. We argue that this mechanism of symmetry breaking underpins observations of colloidal, seed-mediated syntheses of single crystalline metal nanorods capped with strongly interacting surfactants. The parameters within our model are related to experimental observables such as the concentration, hydrophobicity, and binding strength of the surfactants, which suggests a potential route to optimize the yield of asymmetric products in colloidal nanoparticle syntheses.

cond-mat.stat-mech↗

arXiv2024

Atomic evolution of hydrogen intercalation wave dynamics in palladium nanocrystals

Solute-intercalation-induced phase separation creates spatial heterogeneities in host materials, a phenomenon ubiquitous in batteries, hydrogen storage, and other energy devices. Despite many efforts, probing intercalation processes at the atomic scale has been a significant challenge. We study hydrogen (de)intercalation in palladium nanocrystals as a model system and achieve atomic-resolution imaging of hydrogen intercalation wave dynamics by utilizing liquid-phase transmission electron microscopy. Our observations reveal that intercalation wave mechanisms, instead of shrinking-core mechanisms, prevail at ambient temperature for palladium nanocubes ranging from ~60 nm down to ~10 nm. We uncover the atomic evolution of hydrogen intercalation wave transitioning from non-planar and inclined boundaries to those closely aligned with {100} planes. Our kinetic Monte Carlo simulations demonstrate the observed intercalation wave dynamics correspond to sorption pathways minimizing the lattice mismatch strain at the phase boundary. Unveiling the atomic intercalation pathways holds profound implications for engineering intercalation-mediated devices and advancements in energy sciences.

cond-mat.stat-mech↗