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DOE OSTI · 2538340

Simulation of 24,000 Electron Dynamics: Real-Time Time-Dependent Density Functional Theory (TDDFT) with the Real-Space Multigrids (RMG)

Jakowski, Jacek [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000349063574)·Lu, Wenchang [North Carolina State University, Raleigh, NC (United States)]·Briggs, Emil [North Carolina State University, Raleigh, NC (United States)]·Lingerfelt, David [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000256300534)·Sumpter, Bobby G. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000163410355)·Ganesh, Panchapakesan [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000271702902)·Bernholc, Jerzy [North Carolina State University, Raleigh, NC (United States)] (ORCID:0000000299818851)
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Abstract

Here, we present the theory, implementation, and benchmarking of a real-time time-dependent density functional theory (RT-TDDFT) module within the RMG code, designed to simulate the electronic response of molecular systems to external perturbations. Our method offers insights into nonequilibrium dynamics and excited states across a diverse range of systems, from small organic molecules to large metallic nanoparticles. Benchmarking results demonstrate excellent agreement with established TDDFT implementations and showcase the superior stability of our time integration algorithm, enabling long-term simulations with minimal energy drift. The scalability and efficiency of RMG on massively parallel architectures allow for simulations of complex systems, such as plasmonic nanoparticles with thousands of atoms. Future extensions, including nuclear and spin dynamics, will broaden the applicability of this RT-TDDFT implementation, providing a powerful toolset for studies of photoactive materials, nanoscale devices, and other systems where real-time electronic dynamics is essential.

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Jakowski, Jacek [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000349063574), Lu, Wenchang [North Carolina State University, Raleigh, NC (United States)], Briggs, Emil [North Carolina State University, Raleigh, NC (United States)], Lingerfelt, David [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000256300534), Sumpter, Bobby G. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000163410355), Ganesh, Panchapakesan [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000271702902), Bernholc, Jerzy [North Carolina State University, Raleigh, NC (United States)] (ORCID:0000000299818851). 2025-01-23. Simulation of 24,000 Electron Dynamics: Real-Time Time-Dependent Density Functional Theory (TDDFT) with the Real-Space Multigrids (RMG). https://doi.org/10.1021/acs.jctc.4c01241

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