Kinetic Monte Carlo
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RASPA: molecular simulation software for adsorption and diffusion in flexible nanoporous materials Open
A new software package, RASPA, for simulating adsorption and diffusion of molecules in flexible nanoporous materials is presented. The code implements the latest state-of-the-art algorithms for molecular dynamics and Monte Carlo (MC) in va…
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Computational Methods in Heterogeneous Catalysis Open
The unprecedented ability of computations to probe atomic-level details of catalytic systems holds immense promise for the fundamentals-based bottom-up design of novel heterogeneous catalysts, which are at the heart of the chemical and ene…
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Stabilization of Single Metal Atoms on Graphitic Carbon Nitride Open
Graphitic carbon nitride (g‐C 3 N 4 ) exhibits unique properties as a support for single‐atom heterogeneous catalysts (SAHCs). Understanding how the synthesis method, carrier properties, and metal identity impact the isolation of metal cen…
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Atomistic Insights into Nitrogen-Cycle Electrochemistry: A Combined DFT and Kinetic Monte Carlo Analysis of NO Electrochemical Reduction on Pt(100) Open
Electrocatalytic denitrification is a promising technology for the removal of NOx species in groundwater. However, a lack of understanding of the molecular pathways that control the overpotential and product distribution have limited the d…
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A Practical Guide to Surface Kinetic Monte Carlo Simulations Open
This review article is intended as a practical guide for newcomers to the field of kinetic Monte Carlo (KMC) simulations, and specifically to lattice KMC simulations as prevalently used for surface and interface applications. We will provi…
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Dry Reforming of Methane on Single-Site Ni/MgO Catalysts: Importance of Site Confinement Open
Single-site catalysts (SSCs) have drawn considerable attention, because of their superior behaviors in catalysis. However, the origin of promoting the effect of a single site is not well understood. Here in this paper, we take the single-a…
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Roles of Mo Surface Dopants in Enhancing the ORR Performance of Octahedral PtNi Nanoparticles Open
Doping with a transition metal was recently shown to greatly boost the activity and durability of PtNi/C octahedral nanoparticles (NPs) for the oxygen reduction reaction (ORR), but its specific roles remain unclear. By combining electroche…
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Historical review of computer simulation of radiation effects in materials Open
In this Article, I review the development of computer simulation techniques for studying radiation effects in materials from 1946 until 2018. These developments were often closely intertwined with associated experimental developments, whic…
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Formation of active sites on transition metals through reaction-driven migration of surface atoms Open
Adopting low-index single-crystal surfaces as models for metal nanoparticle catalysts has been questioned by the experimental findings of adsorbate-induced formation of subnanometer clusters on several single-crystal surfaces. We used dens…
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Carbon Monoxide Poisoning Resistance and Structural Stability of Single Atom Alloys Open
Platinum group metals (PGMs) serve as highly active catalysts in a variety of heterogeneous chemical processes. Unfortunately, their high activity is accompanied by a high affinity for CO and thus, PGMs are susceptible to poisoning. Alloyi…
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Study of Li atom diffusion in amorphous Li3PO4 with neural network potential Open
To clarify atomic diffusion in amorphous materials, which is important in novel information and energy devices, theoretical methods having both reliability and computational speed are eagerly anticipated. In the present study, we applied n…
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Vacancy-Mediated Anion Photosegregation Kinetics in Mixed Halide Hybrid Perovskites: Coupled Kinetic Monte Carlo and Optical Measurements Open
Solution-processed mixed halide perovskites are excellent materials for multijunction solar cells. Unfortunately, light-induced halide phase segregation has prevented their effective integration into working devices. In this study, we rati…
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First-Principles Statistical Mechanics of Multicomponent Crystals Open
The importance of configurational, vibrational, and electronic excitations in crystalline solids of technological interest makes a rigorous treatment of thermal excitations an essential ingredient in first-principles models of materials be…
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Encounter-Limited Charge-Carrier Recombination in Phase-Separated Organic Semiconductor Blends Open
The theoretical effects of phase separation on encounter-limited charge carrier recombination in organic semiconductor blends are investigated using kinetic Monte Carlo simulations of pump-probe experiments. Using model bulk heterojunction…
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Impact of doping on the density of states and the mobility in organic semiconductors Open
We experimentally investigated conductivity and mobility of poly(3-hexylthiophene) (P3HT) doped with tetrafluorotetracyanoquinodimethane (F(4)TCNQ) for various relative doping concentrations ranging from ultralow (10(-5)) to high (10(-1)) …
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Constant-pH Hybrid Nonequilibrium Molecular Dynamics–Monte Carlo Simulation Method Open
A computational method is developed to carry out explicit solvent simulations of complex molecular systems under conditions of constant pH. In constant-pH simulations, preidentified ionizable sites are allowed to spontaneously protonate an…
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Monte Carlo Study of Real Time Dynamics on the Lattice Open
Monte Carlo studies involving real time dynamics are severely restricted by the sign problem that emerges from a highly oscillatory phase of the path integral. In this Letter, we present a new method to compute real time quantities on the …
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Understanding filamentary growth in electrochemical metallization memory cells using kinetic Monte Carlo simulations Open
A kinetic Monte Carlo model for ECM cells is presented that explains the influence of mechanical stress on filamentary growth.
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Understanding Surface Densified Phases in Ni-Rich Layered Compounds Open
Understanding structural transformation at the surface of Ni-rich layered compounds is of particular importance for improving the performance of these cathode materials. In this Letter, we identify the surface phases using first-principles…
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Nucleation–Elongation Dynamics of Two-Dimensional Covalent Organic Frameworks Open
Homogeneous two-dimensional (2D) polymerization is a poorly understood process in which topologically planar monomers react to form planar macromolecules, often termed 2D covalent organic frameworks (COFs). While these COFs have traditiona…
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Kinetic Monte Carlo simulations for heterogeneous catalysis: Fundamentals, current status, and challenges Open
Kinetic Monte Carlo (KMC) simulations in combination with first-principles (1p)-based calculations are rapidly becoming the gold-standard computational framework for bridging the gap between the wide range of length scales and time scales …
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Machine learning for metallurgy I. A neural-network potential for Al-Cu Open
High-strength metal alloys achieve their performance via careful control of precipitates and solutes. The nucleation, growth, and kinetics of precipitation, and the resulting mechanical properties, are inherently atomic scale phenomena, pa…
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Gas-Phase Synthesis of Trimetallic Nanoparticles Open
To this day, engineering nanoalloys beyond bimetallic compositions has scarcely been within the scope of physical deposition methods due to the complex, nonequilibrium processes they entail. Here, we report a gas-phase synthesis strategy f…
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Accelerated molecular dynamics methods: introduction and recent developments Open
A long-standing limitation in the use of molecular dynamics (MD) simulation is that it can only be applied directly to processes that take place on very short timescales: nanoseconds if empirical potentials are employed, or picoseconds if …
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Cross-kinks control screw dislocation strength in equiatomic bcc refractory alloys Open
Refractory multi-element alloys (RMEA) with body-centered cubic (bcc) structure have been the object of much research over the last decade due to their high potential as candidate materials for high-temperature applications. Most of these …
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Comparing Monte Carlo methods for finding ground states of Ising spin glasses: Population annealing, simulated annealing, and parallel tempering Open
Population annealing is a Monte Carlo algorithm that marries features from simulated-annealing and parallel-tempering Monte Carlo. As such, it is ideal to overcome large energy barriers in the free-energy landscape while minimizing a Hamil…
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Faceting of Equilibrium and Metastable Nanostructures: A Phase-Field Model of Surface Diffusion Tackling Realistic Shapes Open
Several crystalline structures are metastable or kinetically frozen out-of-equilibrium states in the phase space. When the corresponding lifetime is sufficiently long, typical equilibrium features such as regular and extended faceting can …
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Simulating charge transport in organic semiconductors and devices: a review Open
Charge transport simulation can be a valuable tool to better understand, optimise and design organic transistors (OTFTs), photovoltaics (OPVs), and light-emitting diodes (OLEDs). This review presents an overview of common charge transport …
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How Size Matters: Electronic, Cooperative, and Geometric Effect in Perovskite-Supported Copper Catalysts for CO<sub>2</sub> Reduction Open
In heterogeneous catalysis, bifunctional catalysts often outperform one-component catalysts. The activity is also strongly influenced by the morphology, size, and distribution of catalytic particles. For CO2 hydrogenation, the size of the …
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Beyond mean-field approximations for accurate and computationally efficient models of on-lattice chemical kinetics Open
Modeling the kinetics of surface catalyzed reactions is essential for the design of reactors and chemical processes. The majority of microkinetic models employ mean-field approximations, which lead to an approximate description of catalyti…