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Esteban D. Gadea

Publications and source records attributed to Esteban D. Gadea.

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Bridging simulation length scales with cellular automata

Multiscale simulation requires coupling physics models that operate at different characteristic length and time scales, because no single method spans the range needed for most problems of interest. Moving to a coarser-grained representation unlocks longer length and time scales, but it discards the microscopic interactions that build morphology. A fine-grained model can be initialized from an arbitrary packing and left to self-assemble into a physically meaningful structure; a lower-resolution model cannot, and must inherit its starting configuration from a higher-fidelity simulation. The length scales accessible to the coarse-grained model are therefore set not by the coarse-grained method itself, but by the largest fine-grained configuration that can be affordably equilibrated. A representative example is the scale-up from particle-based molecular dynamics (MD) to a lattice-based representation such as kinetic Monte Carlo (kMC). In this work, we present a cellular automata (CA) approach for generating arbitrarily large lattice starting configurations. CA is a natural fit for this task: short-ranged local rules drive the evolution of a lattice, and their repeated application gives rise to emergent long-range order, thematically mirroring how short-ranged interactions in MD produce self-assembled morphology. We use a configuration from a higher-fidelity simulation as a training set and learn the CA rules from it via logistic regression. As a proof of principle, we develop these rules for a hydrated anion exchange membrane (AEM), generate new starting configurations, and benchmark their performance in mesoscale kMC simulations against an MD-derived "ground truth." We then demonstrate the ability to generate substantially larger lattices and show that their behavior in kMC is consistent with that of the smaller CA benchmark configurations.

cond-mat.mtrl-sci

Bias, length, or coupling? What controls the quantum efficiency of electroluminescent single-polymers

Since the first evidence of luminescence of organic polymers in STM junctions, efforts have been invested in elucidating how to leverage the voltage, anchoring chemistry, and molecular structure to optimize emission power and efficiency. Understanding the fundamentals underlying current-driven molecular emission is important not only for OLED engineering, but also to control luminescence at the atomic scale toward the mastering of single or localized photon sources. However, the difficulty in isolating the separate roles of the variables at play in molecular junction experiments, has precluded a general comprehension of their distinctive effects on the emitted power and the quantum yield. In the present report, we use time-dependent electronic structure simulations based on quantum electrodynamics to disentangle the incidence of bias, electronic coupling and molecular length on device performance, with polyphenylene-vinylene as a case study. A careful validation demonstrates that our approach can achieve quantitative agreement with available experimental data. Through its application we identify the applied bias as the main factor determining emission power. The quantum efficiency, however, is influenced only minimally by bias and electronic coupling, and is instead dominated by polymer length, on which it depends exponentially. Thus, using longer polymer chains emerges as the primary strategy for achieving higher efficiencies. Our results thereby provide key prescriptions for designing single-molecule electroluminescent platforms.

cond-mat.mtrl-sci