Many-Body Methods, Spectroscopies, and Dynamics for Molecular Polaritonic Systems
Light when nanoconfined in cavities and made to interact strongly with molecules results in hybrid light–matter states or polaritons, which can be used to modify and manipulate ground and excited-state potential energy surfaces and thus alter the reactivity and energy flow profoundly in molecular systems.The development of predictive theories for molecular polaritons requires combining electronic degrees of freedom, as provided by quantum chemistry methods, with quantum electrodynamics (QED) treatments of the photonic degrees of freedom.
Our vision is to develop a suite of theoretical frameworks, spanning low-order to high-level many-body methods, that will provide unprecedented ability to capture the structure and dynamics of molecular polaritonic systems and deliver scalable software source code and libraries that can harness leadership-class computational facilities (LCFs). In pursuit of this vision, we have three project objectives to guide our research program, which was initiated in September 2022.
- Objective 1: Develop a Gaussian basis set–based suite of methods spanning low-order to high-level ab initio many-body approaches for modeling and simulation of molecular polaritonic systems.
- Objective 2: Implement polaritonic many-body methods to fully utilize modern heterogeneous (CPU/GPU) high-performance computing platforms at DOE’s LCFs.
- Objective 3: Apply developed methods to molecular polaritonic systems to validate, benchmark, and assess our developments with reference systems, progressing to advanced applications to complement experiments to enhance fundamental understanding of polaritonic chemistry.
Funding
The Center for Many-Body Methods, Spectroscopies, and Dynamics for Molecular Polaritonic Systems (MAPOL) is funded under FWP 79715 as part of the Computational Chemical Sciences (CCS) program by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences at Pacific Northwest National Laboratory (PNNL). PNNL is a multiprogram national laboratory operated by Battelle Memorial Institute for the United States Department of Energy under DOE contract number DE-AC05-76RL1830.