Ultrafast Near-Edge X-ray Absorption Fine Structure Calculations with the Exact Integral Simplified Time-Dependent Density Functional Theory (XsTD-DFT) for Large Systems
(2025) Journal of Physical Chemistry Letters — n° 16, p. 13132-13138 (2025)
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- Computing a near-edge X-ray absorption fine structure (NEXAFS) is a real challenge for quantum chemistry (QC), as for medium to large systems, it involves a high density of core–valence excited states. With the boundaries of QC pushed at its maximum with the exact integral simplified time-dependent density functional theory (XsTD-DFT) framework, an ultrafast method is proposed to compute such excitations with short-range corrected exchange–correlation functionals using the Tamm–Dancoff approximation. For small to medium size systems, computations were performed in less than a minute, providing striking comparisons with respect to the experiment. To showcase the performance of the method, the computed oxygen K-edge NEXAFS spectrum for a collagen model of 600 atoms was compared to the experimental spectrum of collagen. Computing 85 672 1sO core–valence excited states was necessary to reproduce the experimental spectrum. The calculation took only 11 days on a desktop computer. With knowledge of the simplicity of this “small” static model of collagen, the comparison to the experiment remains excellent.
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de Wergifosse, M. (2025). Ultrafast Near-Edge X-ray Absorption Fine Structure Calculations with the Exact Integral Simplified Time-Dependent Density Functional Theory (XsTD-DFT) for Large Systems. Journal of Physical Chemistry Letters, 16, 13132-13138. https://doi.org/10.1021/acs.jpclett.5c03411 (Original work published 2025)