A New Kinetic Monte Carlo Algorithm for Heteroepitactical Growth: Case Study of C<sub>60</sub> Growth on Pentacene

Cantrell, Rebecca; Clancy, Paulette

doi:10.1021/ct200819r

Cited by 12 publications

(14 citation statements)

References 23 publications

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“…In comparison to previous estimates we find that our value for the free diffusion barrier of E D = 195.6 (20) meV falls between the values obtained previously: Gravil et al [30] (168 meV, pair potential calculations), Liu et al [19] (178(4) meV, MD simulations), Cantrell and Clancy [24] (205( 22) meV, molecular mechanics), and Goose et al [23] (207 meV, DFT calculations). In Table II, we compare our values for energy barriers to available previous results.…”

Section: A MD Simulationssupporting

confidence: 82%

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Modeling epitaxial film growth of C$_{60}$ revisited

Janke,

Speck

2020

Preprint

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Epitaxial films evolve on time and length scales that are inaccessible to atomistic computer simulation methods like molecular dynamics (MD). To numerically predict properties for such systems, a common strategy is to employ kinetic Monte Carlo (KMC) simulations, for which one needs to know the transition rates of the involved elementary steps. The main challenge is thus to formulate a consistent model for the set of transition rates and to determine its parameters. Here we revisit a well-studied model system, the epitaxial film growth of the fullerene C60 on an ordered C60 substrate(111). We implement a systematic multiscale approach in which we determine transition rates through MD simulations of specifically designed initial configurations. These rates follow Arrhenius' law, from which we extract energy barriers and attempt rates. We discuss the issue of detailed balance for the resulting rates. Finally, we study the morphology of subatomic and multilayer film growth and compare simulation results to experiments. Our model enables further studies on multi-layer growth processes of C60 on other substrates.

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Section: A MD Simulationssupporting

confidence: 82%

“…One approach is to assume an Arrhenius law, which requires an attempt rate and an energy barrier for each possible transition. For C 60 , energy barriers have been calculated from density functional theory (DFT) [23] and molecular mechanics [24].…”

Section: Introductionmentioning

confidence: 99%

Modeling epitaxial film growth of C$_{60}$ revisited

Janke,

Speck

2020

Preprint

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“…KMC uses a library of known transitions to study multilayer surface growth. Since standard KMC codes are unsuited to study heteroepitactic growth, we previously developed an algorithm tailored to do so and hence follow the growth of C 60 on pentacene . The algorithm featured a multilattice framework with a seamless ability to switch “grids” from those suitable for pentacene and C 60 to match the selected event.…”

Section: Methodsmentioning

confidence: 99%

“…(In contrast, heteroepitaxy concerns situations in which A and B materials share the same preferred crystal habit (e.g., Si on Ge).) There have been just two prior reports of KMC simulation of heteroepitactic growth; one uses a multilattice KMC method we created and applied to submonolayer growth . In the second, Hoffman investigated how environmental conditions of a CO molecule on a Pd (100) surface (e.g., different adsorption site geometries) determined which of the two lattices (CO or Pd) it adopted .…”

Section: Introductionmentioning

confidence: 99%

Multiscale Simulation and Modeling of Multilayer Heteroepitactic Growth of C₆₀ on Pentacene

et al. 2016

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We apply multiscale methods to describe the strained growth of multiple layers of C60 on a thin film of pentacene. We study this growth in the presence of a monolayer pentacene step to compare our simulations to recent experimental studies by Breuer and Witte of submonolayer growth in the presence of monolayer steps. The molecular-level details of this organic semiconductor interface have ramifications on the macroscale structural and electronic behavior of this system and allow us to describe several unexplained experimental observations for this system. The growth of a C60 thin film on a pentacene surface is complicated by the differing crystal habits of the two component species, leading to heteroepitactical growth. In order to probe this growth, we use three computational methods that offer different approaches to coarse-graining the system and differing degrees of computational efficiency. We present a new, efficient reaction-diffusion continuum model for 2D systems whose results compare well with mesoscale kinetic Monte Carlo (KMC) results for submonolayer growth. KMC extends our ability to simulate multiple layers but requires a library of predefined rates for event transitions. Coarse-grained molecular dynamics (CGMD) circumvents KMC's need for predefined lattices, allowing defects and grain boundaries to provide a more realistic thin film morphology. For multilayer growth, in this particularly suitable candidate for coarse-graining, CGMD is a preferable approach to KMC. Combining the results from these three methods, we show that the lattice strain induced by heteroepitactical growth promotes 3D growth and the creation of defects in the first monolayer. The CGMD results are consistent with experimental results on the same system by Conrad et al. and by Breuer and Witte in which C60 aggregates change from a 2D structure at low temperature to 3D clusters along the pentacene step edges at higher temperatures.

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“…One route to further our understanding is computer simulations. Especially the kinetic Monte Carlo (KMC) method [33] (or Gillespie algorithm [34,35]) has proven to be very promising since it is able to simulate the length and time scales needed to observe the cluster growth of these deposition experiments [36][37][38][39][40][41][42].…”

Section: Introductionmentioning

confidence: 99%

Multiscale modelling of structure formation of C$_{60}$ on insulating CaF$_2$ substrates

Janke,

Speck

2021

Preprint

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Morphologies of adsorbed molecular films are of interest in a wide range of applications. To study the epitaxial growth of these systems in computer simulations requires access to long time and length scales and one typically resorts to kinetic Monte Carlo (KMC) simulations. However, KMC simulations require as input transition rates and their dependence on external parameters (such as temperature). Experimental data allows only limited and indirect access to these rates, and models are often oversimplified. Here we follow a bottom-up approach and aim to systematically construct all relevant rates for an example system that has shown interesting properties in experiments, buckminsterfullerene on a calcium fluoride substrate. We develop classical force fields (both atomistic and coarse-grained) and perform molecular dynamics simulations of the elementary transitions in order to derive explicit expressions for the transition rates with a minimal number of free parameters.

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A New Kinetic Monte Carlo Algorithm for Heteroepitactical Growth: Case Study of C₆₀ Growth on Pentacene

Cited by 12 publications

References 23 publications

Modeling epitaxial film growth of C$_{60}$ revisited

Modeling epitaxial film growth of C$_{60}$ revisited

Multiscale Simulation and Modeling of Multilayer Heteroepitactic Growth of C₆₀ on Pentacene

Multiscale modelling of structure formation of C$_{60}$ on insulating CaF$_2$ substrates

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A New Kinetic Monte Carlo Algorithm for Heteroepitactical Growth: Case Study of C60 Growth on Pentacene

Cited by 12 publications

References 23 publications

Modeling epitaxial film growth of C$_{60}$ revisited

Modeling epitaxial film growth of C$_{60}$ revisited

Multiscale Simulation and Modeling of Multilayer Heteroepitactic Growth of C60 on Pentacene

Multiscale modelling of structure formation of C$_{60}$ on insulating CaF$_2$ substrates

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A New Kinetic Monte Carlo Algorithm for Heteroepitactical Growth: Case Study of C₆₀ Growth on Pentacene

Multiscale Simulation and Modeling of Multilayer Heteroepitactic Growth of C₆₀ on Pentacene