Simanta Lahkar | Searcharxiv

arXiv2025

Decoupling Electric Field and Temperature-Driven Atomistic Forming Mechanisms in TaOx/HfO2-Based ReRAMs using Reactive Molecular Dynamics Simulations

Resistive random access memories (ReRAMs) with a bilayer TaOx/HfO2 stack structure have shown unique multi-level resistive switching capabilities. However, the physical processes governing their behavior, and specifically the atomistic mechanisms of forming, remain poorly understood. In this work, we present a detailed analysis of the forming mechanism at the atomic level using molecular dynamics (MD) simulations. An extended charge equilibration scheme, based on a combination of the charge transfer ionic potential (CTIP) formalism and the electrochemical dynamics with implicit degrees of freedom (EChemDID) method, is employed to model the localized effects of applied voltage. Our simulations reveal that tantalum ions exhibit the highest displacement under applied voltage, followed by hafnium ions, while oxygen ions respond only minimally. This results in the formation of a tantalum-depleted, oxygen-rich zone near the positive top electrode (anode), and the clustering of oxygen vacancies near the negative bottom electrode (cathode), where the conductive filament nucleates. This ionic segregation partially shields the bulk dielectric from the applied electric field, hindering further migration of ions in the vertical direction. We find that a minimum threshold voltage is required to initiate vacancy clustering. Filament growth proceeds through a localized mechanism, driven by thermally activated generation of oxygen vacancy defects, which are stabilized near the edge of the nucleated filament at the cathode.

cond-mat.mtrl-sci↗

arXiv2023

Competing mechanisms govern the thermal rectification behavior in semi-stochastic polycrystalline graphene with graded grain-size distribution

Thermal rectifiers are devices that have different thermal conductivities in opposing directions of heat flow. The realization of practical thermal rectifiers relies significantly on a sound understanding of the underlying mechanisms of asymmetric heat transport, and two-dimensional materials offer a promising opportunity in this regard owing to their simplistic structures together with a vast possibility of tunable imperfections. However, the in-plane thermal rectification mechanisms in 2D materials like graphene having directional gradients of grain sizes have remained elusive. In fact, understanding the heat transport mechanisms in polycrystalline graphene, which are more practical to synthesize than large-scale single-crystal graphene, could potentially allow a unique opportunity, in principle, to combine with other defects and designs for effective optimization of thermal rectification. In this work, we investigate the thermal rectification behavior in periodic atomistic models of polycrystalline graphene whose grain arrangements were generated semi-stochastically to have different gradient grain-density distributions along the in-plane heat flow direction. We employ the centroidal Voronoi tessellation technique to generate realistic grain boundary structures for graphene, and the non-equilibrium molecular dynamics simulations method is used to calculate the thermal conductivities and rectification values. Additionally, detailed phonon characteristics and propagating phonon spatial energy densities are analyzed based on the fluctuation-dissipation theory to elucidate the competitive interplay between two underlying mechanisms, namely, (1) propagating phonon coupling and (2) temperature-dependence of thermal conductivity that determine the degree of asymmetric heat flow in graded polycrystalline graphene.

cond-mat.mtrl-sci↗