Quantum Electrodynamics Coupled-Cluster at Scale: High-Performance Implementation for Complex Systems

Area of Science:

• Quantum chemistry
• Computational physics
• Chemical reaction dynamics

Background:

• Coupled-cluster (CC) theory accurately simulates quantum systems.
• Quantum electrodynamics (QED) extends CC theory to model electron-photon interactions, enabling cavity-modified chemistry.
• Simulating larger systems with QED-CC is computationally expensive and lacks scalable infrastructure.

Purpose of the Study:

• To present a GPU-enabled, high-performance, open-source implementation of QED-CC with single and double excitations (QED-CCSD).
• To integrate QED-CCSD into the ExaChem quantum chemistry software package using the TAMM infrastructure.
• To demonstrate the capability of simulating larger systems and analyzing the impact of photonic degrees-of-freedom on ground-state properties.

Main Methods:

• Developed a GPU-enabled QED-CCSD implementation.
• Utilized the Tensor Algebra for Many-body Methods (TAMM) for scalable performance on heterogeneous supercomputing platforms.
• Performed numerical benchmarks to validate the implementation and assess scalability.

Main Results:

• Successfully implemented and validated a GPU-accelerated QED-CCSD method within ExaChem.
• Demonstrated the ability to simulate larger quantum systems than previously possible with QED-CC methods.
• Showcased how incorporating photonic degrees-of-freedom influences the ground-state properties of simulated systems.

Conclusions:

• The developed QED-CCSD implementation provides a scalable and efficient approach for simulating cavity-modified chemistry.
• ExaChem, powered by TAMM, offers a robust platform for high-performance quantum electrodynamics coupled-cluster calculations.
• This advancement facilitates accurate predictions of chemical reactions influenced by light-matter interactions in larger, more complex systems.