957 lines
81 KiB
Text
957 lines
81 KiB
Text
<!DOCTYPE html>
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<h1 class="nist-page__title">Multi-code Benchmark on Ti K-edge X-ray Absorption Spectra of Ti-O Compounds</h1>
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<div class="nist-field__label">Published</div>
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<div class="nist-field__item"><time datetime="2024-01-11T12:00:00Z">January 11, 2024</time>
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<h3 class="nist-field__label">Author(s)</h3>
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<div class="nist-field__item">Fanchen Meng, Benedikt Maurer, Fabian Peschel, Sencer Selcuk, Xiaohui Qu, Mark S Hybertsen, Christian Vorwerk, Claudia Draxl, <span class="nist-author">John Vinson</span>, Deyu Lu</div>
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<h3>Abstract</h3>
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X-ray absorption spectroscopy (XAS) is an element-specific materials characterization technique that is sensitive to structural and electronic properties. First-principles simulated XAS has been widely used as a powerful tool to interpret experimental spectra and draw physical insights. Recently, there has also been growing interest in building computational XAS databases to enable data analytics and machine learning applications. However, there are non-trivial differences among commonly used XAS simulation codes, both in underlying theoretical formalism and in technical implementation. Reliable and reproducible computational XAS databases require systematic benchmark studies. In this work, we benchmarked Ti K-edge XAS simulations of ten representative Ti-O binary compounds, which we refer to as the Ti-O-10 dataset, using three state-of-the-art codes: \xs}, \ocean} and \exciting}. We systematically studied the convergence behavior with respect to the input parameters and developed a workflow to automate and standardize the calculations to ensure converged spectra. Our benchmark comparison considers a 35 eV spectral range starting from the K-edge onset, representative of widely used near-edge spectra. Quantitative comparison over this range is based on Spearman's rank correlation score ($r_sp}$). Our results show: (1) the two Bethe-Salpeter equation (BSE) codes (\ocean} and \exciting}) have excellent agreement with an average $r_sp}$ of 0.998; (2) good agreement is obtained between the core-hole potential code (\xs}) and BSE codes (\ocean} and \exciting}) with an average $r_sp}$ of 0.990, and this smaller $r_sp}$ reflects the noticeable differences in the main edge spectral shape that can be primarily attributed to the difference in the strength of the screened core-hole potential; (3) simulations from both methods overall reproduce well the main experimental spectral features of rutile and anatase, and the different treatments of the screened core-hole potential have visible impact on pre-edge intensities and the peak ratio of the main edge; (4) there exist moderate differences in the relative edge alignment of the three codes with a standard deviation of about 0.2 eV, which arise from multiple contributions including the frozen core approximation, final state effects, and different approximations used for the self-energy correction. Our benchmark study provides important standards for first-principles XAS simulations with broad impact in data-driven XAS analysis.
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<div class="nist-field__item">Physical Review Materials</div>
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Meng, F.
|
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, Maurer, B.
|
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, Peschel, F.
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, Selcuk, S.
|
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, Qu, X.
|
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, Hybertsen, M.
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, Vorwerk, C.
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, Draxl, C.
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, Vinson, J.
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and Lu, D.
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(2024),
|
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Multi-code Benchmark on Ti K-edge X-ray Absorption Spectra of Ti-O Compounds, Physical Review Materials, [online], https://doi.org/10.1103/PhysRevMaterials.8.013801, https://tsapps.nist.gov/publication/get_pdf.cfm?pub_id=935456
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(Accessed March 4, 2025)
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Created January 11, 2024, Updated January 31, 2024
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