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Overall, our work demonstrates the importance of using multiple force-field and sampling method combinations for accurate structural and thermodynamic information in the study of disordered proteins.Simple arguments based on orbital energies and crystal symmetry suggest the band gap of CsTaS3 to be suitable for solar cell photovoltaics. Here, we combine chemical theory with sophisticated calculations to describe an intricate relationship between the structure and optical properties of this material. Orbital interactions govern both the

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