X-ray photoelectron spectroscopy (XPS) is a powerful characterization technique that unveils subtle chemical environment differences via core– electron binding energy (CEBE) analysis. We extend the development of realspace pseudopotential methods to calculating 1s, 2s, and 2p3/2 CEBEs of third-row elements (S, P, and Si) within the framework of Kohn–Sham density-functional theory (KS-DFT). The new approach systematically prevents variational collapse and simplifies core-excited orbital selection within dense energy level distributions. However, careful error cancellation analysis is required to achieve accuracy comparable to all-electron methods and experiments. Combined with real-space KS-DFT implementation, this development enables large-scale simulations with both Dirichlet boundary conditions and periodic boundary conditions.
Liu, Liping, et al. "Real-Space Pseudopotential Method for the Calculation of Third-Row Elements X-ray Photoelectron Spectroscopic Signatures." Journal of Chemical Theory and Computation, vol. 20, no. 14, Jul. 2024. https://doi.org/10.1021/acs.jctc.4c00535
Liu, Liping, Xu, Qiang, dos Anjos Cunha, Leonardo, Xin, Hongliang, Head-Gordon, Martin, & Qian, Jin (2024). Real-Space Pseudopotential Method for the Calculation of Third-Row Elements X-ray Photoelectron Spectroscopic Signatures. Journal of Chemical Theory and Computation, 20(14). https://doi.org/10.1021/acs.jctc.4c00535
Liu, Liping, Xu, Qiang, dos Anjos Cunha, Leonardo, et al., "Real-Space Pseudopotential Method for the Calculation of Third-Row Elements X-ray Photoelectron Spectroscopic Signatures," Journal of Chemical Theory and Computation 20, no. 14 (2024), https://doi.org/10.1021/acs.jctc.4c00535
@article{osti_2395988,
author = {Liu, Liping and Xu, Qiang and dos Anjos Cunha, Leonardo and Xin, Hongliang and Head-Gordon, Martin and Qian, Jin},
title = {Real-Space Pseudopotential Method for the Calculation of Third-Row Elements X-ray Photoelectron Spectroscopic Signatures},
annote = {X-ray photoelectron spectroscopy (XPS) is a powerful characterization technique that unveils subtle chemical environment differences via core– electron binding energy (CEBE) analysis. We extend the development of realspace pseudopotential methods to calculating 1s, 2s, and 2p3/2 CEBEs of third-row elements (S, P, and Si) within the framework of Kohn–Sham density-functional theory (KS-DFT). The new approach systematically prevents variational collapse and simplifies core-excited orbital selection within dense energy level distributions. However, careful error cancellation analysis is required to achieve accuracy comparable to all-electron methods and experiments. Combined with real-space KS-DFT implementation, this development enables large-scale simulations with both Dirichlet boundary conditions and periodic boundary conditions.},
doi = {10.1021/acs.jctc.4c00535},
url = {https://www.osti.gov/biblio/2395988},
journal = {Journal of Chemical Theory and Computation},
issn = {ISSN 1549-9618},
number = {14},
volume = {20},
place = {United States},
publisher = {American Chemical Society},
year = {2024},
month = {07}}
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
National Science Foundation (NSF); US Department of Energy; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Chemical Sciences, Geosciences & Biosciences Division (SC-22.1); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
AC02-05CH11231; SC0021266
OSTI ID:
2395988
Alternate ID(s):
OSTI ID: 2406184 OSTI ID: 2568336
Journal Information:
Journal of Chemical Theory and Computation, Journal Name: Journal of Chemical Theory and Computation Journal Issue: 14 Vol. 20; ISSN 1549-9618
Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 268, Issue 1184https://doi.org/10.1098/rsta.1970.0060