Center for Computational Study of Excited-State Phenomena in Energy Materials

Steven Louie, Director

The discovery and development of new functional architectures for harvesting, converting, and storing energy is at present significantly limited by our understanding of how integrated complex material components assemble and transduce energy. Predictions of the behavior of such systems require going beyond ground-state properties, to excited states and dynamics, and associated structural and orbital relaxations in the excited state. While public domain software is widely available and used to search for materials with desirable ground-state properties, similar tools for excited states (e.g., electronic spectra, optical responses, fast electron dynamics, etc.) are still nascent, particularly for complex systems. The lack of scalable, versatile, and user-friendly software for excited-state properties has been a major roadblock for the design of functional materials for energy applications. The objective of the program is to develop general software, incorporating new methods and theories, to elucidate and predict excited-state phenomena in energy-related materials.

Our software will use advanced algorithms and first-principles many-body perturbation theory that fully include but also go well beyond the interacting one- and two-particle Green's functions to compute electron excitations and lifetimes, optical spectra, exciton-exciton interactions, trion formation, nonlinear optical processes, excited-state decay, pump-probe fast dynamics, and more. Currently, there exists no first-principles methodology or general software for prediction of phenomena beyond 2-particle correlated excitations in materials. The methods and software developed will be highly relevant to complex materials for energy applications and be validated through close collaboration with experimental groups. We will develop codes to fully utilize the current petascale and future exascale capabilities of the Department of Energy's high performance computers. We have assembled a team consisting of physical scientists, applied mathematicians, computational scientists, and experimentalists, with complementary expertise, to address this challenge. The end result will be an integrated open-source software package with unique capabilities to predict and understand a variety of excited-state phenomena in complex functional energy materials from first principles with exascale performance.

Please visit the C2SEPEM website to learn more.