Detail

Data-driven Low-rank Approximation for Electron-hole Kernel and Acceleration of Time-dependent GW Calculations

Hou, Bowen; Wu, Jinyuan; Lee, Victor Chang; Guo, Jiaxuan; Liu, Luna Y.; Qiu, Diana Y.

Year

2025

Source Name

e32dae46-863d-4c13-a9ef-a36eefa38a78

License

Creative Commons Attribution 4.0

Contacts

Bowen Hou (bowen.hou@yale.edu)

DOI

10.18126/1f89-fc48 View on Datacite
Many-body electron-hole interactions are essential for understanding non-linear optical processes and ultrafast spectroscopy of materials. Recent first principles approaches based on nonequilibrium Green’s function formalisms, such as the time-dependent adiabatic GW (TD-aGW) approach, can predict the nonequilibrium dynamics of excited states including electron-hole interactions. However, the high dimensionality of the electron-hole kernel poses significant computational challenges for scalability. Here, we develop a data-driven low-rank approximation for the electron-hole kernel, leveraging localized excitonic effects in the Hilbert space of crystalline systems. Through singular value decomposition (SVD) analysis, we show that the subspace of non-zero singular values, containing the key information of the electron-hole kernel, retains a small size even as the k-grid grows, ensuring computational feasibility with extremely dense k-grids for converged calculations. Utilizing this low-rank property, we achieve at least 95% compression of the kernel and an orderof-magnitude speedup of TD-aGW calculations. Our method, rooted in physical interpretability, outperforms existing machine learning approaches by avoiding intensive training processes and eliminating time-accumulated errors, providing a general framework for high-throughput, nonequilibrium simulation of light-driven dynamics in materials. This dataset includes all the raw data of MoS2 BSE kernel from BerkeleyGW, the TD-aGW generated data, and post-processed data used for plot.