Functional layered materials (LMs) will dominate nanomaterials science in this century. The attractiveness of LMs lies not only in their outstanding electronic, optical, magnetic, and chemical properties, but also in the possibility of tuning these properties in desired ways by building van der Waals heterostructures composed of unlimited combinations of atomically thin layers. For this INCITE project, researchers will perform 10,000-atom nonadiabatic quantum molecular dynamics (NAQMD) and billion-atom reactive molecular dynamics (RMD) simulations for computational synthesis and characterization of revolutionary LMs.

These simulations will (1) aid the synthesis of stacked LMs by chemical vapor deposition, exfoliation, and intercalation; and (2) discover function-property-structure relationships in LMs with a special focus on far-from-equilibrium electronic processes.

This team has already performed the largest-ever RMD and quantum molecular dynamics (QMD) simulations on Mira by fully exploiting the system’s core architecture. For this project, they have designed simulation engines that will continue to scale on future computing platforms based on a common algorithmic framework called divide-conquer-recombine, significantly reducing computational cost in QMD and increasing accuracy in RMD simulations. 

Results will provide predictive theory, directly validated by ultrafast X-ray laser experiments at Stanford’s Linac Coherent Light Source (LCLS), to form a cornerstone of DOE's layered materials genome efforts. Function-property-structure relationships in stacked LMs span a wide range of length and time scales. Together, the simulations and LCLS X-ray laser experiments will, for the first time, describe non-equilibrium dynamics in LMs at exactly the same spatiotemporal scales.