Nuclear Quantum Effects in the Acetylene:Ammonia Plastic Co-crystal (2310.00480v1)

Abstract: Organic molecular solids can exhibit rich phase diagrams. In addition to structurally unique phases, translational and rotational degrees of freedom can melt at different state points, giving rise to partially disordered solid phases. The structural and dynamic disorder in these materials can have a significant impact on the physical properties of the organic solid, necessitating a thorough understanding of disorder at the atomic scale. When these disordered phases form at low temperatures, especially in crystals with light nuclei, the prediction of materials properties can be complicated by the importance of nuclear quantum effects. As an example, we investigate nuclear quantum effects on the structure and dynamics of the orientationally-disordered, translationally-ordered plastic phase of the acetylene:ammonia (1:1) co-crystal that is expected to exist on the surface of Saturn's moon Titan. Titan's low surface temperature (~90 K) suggests that the quantum mechanical behavior of nuclei may be important in this and other molecular solids in these environments. By using neural network potentials combined with ring polymer molecular dynamics simulations, we show that nuclear quantum effects increase orientational disorder and rotational dynamics within the acetylene:ammonia (1:1) co-crystal by weakening hydrogen bonds. Our results suggest that nuclear quantum effects are important to accurately model molecular solids and their physical properties in low temperature environments.