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Data and materials availability: All data are available in the manuscript or supplementary information. All materials are available upon request to L.D. Methods Solution-phase synthesis of pure 2D halide perovskite sheets In this study, ten types of pure 2D halide perovskite sheets were synthesized via a quaternary solvent method.

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Developing accurate coarse-grained (CG) models is critical for addressing long time and length scale phenomena with molecular simulations. Here, we distinguish and quantify two sources of error that are relevant to CG models in order to guide further methods development: “representability” errors, which result from the finite basis associated with the chosen functional form of the CG model and mapping operator, and “information” errors, which result from the limited kind and quantity of data supplied to the CG parameterization algorithm. We have performed a systematic investigation of these errors by generating all possible CG models of three liquids (butane, 1-butanol, and 1,3-propanediol) that conserve a set of chemically motivated locality and topology relationships. In turn, standard algorithms (iterative Boltzmann inversion, IBI, and multiscale coarse-graining, MSCG) were used to parameterize the models and the CG predictions were compared with atomistic results. For off-target properties, we observe a strong correlation between the accuracy and the resolution of the CG model, which suggests that the approximations represented by MSCG and IBI deteriorate with decreasing resolution. Conversely, on-target properties exhibit an extremely weak resolution dependence that suggests a limited role of representability errors in model accuracy. Taken together, these results suggest that simple CG models are capable of utilizing more information than is provided by standard parameterization algorithms, and that model accuracy can be improved by algorithm development rather than resorting to more complicated CG models.

Polymethine dyes in dilute solutions show many of the electronic and optical properties required for all-optical switching applications. However, in the form of thin films, their aggregation and interactions with counterions do generally strongly limit their utility. Here, we present a theoretical approach combining molecular-dynamics simulations and quantum-chemical calculations to describe the bulk molecular packing of streptocyanines (taken as representative of simple polymethines) with counterions of different hardness (Cl − and BPh 4 −) and understand the impact on the optical properties. The accuracy of the force field we use is verified by reproducing experimental crystal parameters as well as the configurations of polymethine/counterion complexes obtained from electronicstructure calculations. The aggregation characteristics can be understood in terms of both polymethine−counterion and polymethine−polymethine interactions. The counterions are found to localize near one end of the streptocyanine backbones, and the streptocyanines form a broad range of aggregates with significant electronic couplings between neighboring molecules. As a consequence, the linear and nonlinear optical properties are substantially modified in the bulk. By providing an understanding of the relationship between the molecular interactions and the bulk optical properties, our results point to a clear strategy for designing polymethine and counterion molecular structures and optimizing the materials properties for all-optical switching applications.