Steering the Quantum Dynamics of Confined Molecular Materials

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Molecular materials are often present in forefront technologies targeting new sustainable energy alternatives. However, most of these alternatives currently fall short of the needs of industry and society. QUADYMM will investigate new fundamental mechanisms that could lead to paradigmatic changes in the design of such technologies. We will explore two main thematic avenues, from a theoretical perspective: 1) tuning the atomic and electronic properties of molecular materials in confined structured environments, and 2) realizing nonequilibrium molecular material states for dynamic control of stable and reactive phases of matter. From a large pool of areas where these concepts can be applied, QUADYMM will focus on water interfaces with inorganic materials and on aromatic hydrocarbon interfaces with 2D materials, because of their fundamental impact on electrochemistry and optoelectronics. The state of the art of computer simulation in this area is still based on classical mechanics of nuclei or simplified models, especially for nonequilibrium and nonadiabatic processes. Once successful, QUADYMM will provide new first-principles methodology to treat electronic and nuclear nonequilibrium dynamics, changing the predictive capacity of computational simulations of important processes, such as water-splitting and vibronic energy transport. Crucially, we will develop novel protocols for the inclusion of external stimuli in quantum dynamics simulations, bridging electronic and vibrational time scales and reaching the thermodynamic limit. This will be achieved by new techniques joining machine-learning methods with first-principles electronic structure and trajectory-based path-integral approaches. The resulting framework will elucidate the nonequilibrium quantum dynamics of complex weakly-bound systems containing thousands of atoms, and provide new structural and electronic phase diagrams to aid vibrational design.