Practical density-corrected density functional theory (DC-DFT) calculations rely on Hartree-Fock (HF) densities, which can be computationally expensive for systems with over a hundred atoms. We extend the applicability of HF-DFT using the dual-basis method, where the density matrix from a smaller basis set is used to estimate the HF solution on a larger basis set. Benchmarks on many systems, including the GMTKN55 database for main-group chemistry, and the L7 and S6L data sets for large molecular systems demonstrate the efficacy of our approach. We apply the dual-basis method to both DNA and HIV systems and compare with the literature. The details of a recent reparameterization of HF-rSCAN-DC4 are explained, showing no loss of performance.
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http://dx.doi.org/10.1021/acs.jpclett.4c02852 | DOI Listing |
J Phys Chem Lett
January 2025
Department of Chemistry, Yonsei University, 50 Yonsei-ro, Seodaemun-gu, Seoul 03722, Korea.
Practical density-corrected density functional theory (DC-DFT) calculations rely on Hartree-Fock (HF) densities, which can be computationally expensive for systems with over a hundred atoms. We extend the applicability of HF-DFT using the dual-basis method, where the density matrix from a smaller basis set is used to estimate the HF solution on a larger basis set. Benchmarks on many systems, including the GMTKN55 database for main-group chemistry, and the L7 and S6L data sets for large molecular systems demonstrate the efficacy of our approach.
View Article and Find Full Text PDFJ Chem Theory Comput
August 2024
Department of Chemistry, Yonsei University, 50 Yonsei-ro Seodaemun-gu, Seoul 03722, Korea.
Almost all empirical parametrizations of dispersion corrections in DFT use only energy errors, thereby mixing functional and density-driven errors. We introduce density and dispersion-corrected DFT (DC-DFT), a dual-calibration approach that accounts for density delocalization errors when parametrizing dispersion interactions. We simply exclude density-sensitive reactions from the training data.
View Article and Find Full Text PDFActa Crystallogr E Crystallogr Commun
August 2024
Centre for Hyperpolarisation in Magnetic Resonance, University of York, Heslington, United Kingdom, YO10 5NY.
Single crystals of the mol-ecular compound, {CuIrCl(CHN)(CHN)]·3.18CHOH or [({CuIr}Cl(IMes)(pyrazine))(pyrazine)]·3.18CHOH [where IMes is 1,3-bis-(2,4,6-trimethylphen-yl)imidazol-2-yl-idene], with a unique heterometallic cluster have been prepared and the structure revealed using single-crystal X-ray diffraction.
View Article and Find Full Text PDFNat Commun
February 2024
The Australian Centre for Excellence in Antarctic Science, University of Tasmania, Hobart, TAS, 7001, Australia.
In recent sea level studies, discrepancies have arisen in ocean mass observations obtained from the Gravity Recovery and Climate Experiment and its successor, GRACE Follow-On, with GRACE estimates consistently appearing lower than density-corrected ocean volume observations since 2015. These disparities have raised concerns about potential systematic biases in sea-level observations, with significant implications for our understanding of this essential climate variable. Here, we reconstruct the global and regional ocean mass change through models of ice and water mass changes on land and find that it closely aligns with both GRACE and density-corrected ocean volume observations after implementing recent adjustments to the wet troposphere correction and halosteric sea level.
View Article and Find Full Text PDFMagn Reson Med
March 2024
Department of Medical Physics and Biomedical Engineering, Centre for Medical Image Computing (CMIC), University College London, London, UK.
Purpose: To demonstrate proof-of-concept of a T *-sensitized oxygen-enhanced MRI (OE-MRI) method at 3T by assessing signal characteristics, repeatability, and reproducibility of dynamic lung OE-MRI metrics in healthy volunteers.
Methods: We performed sequence-specific simulations for protocol optimisation and acquired free-breathing OE-MRI data from 16 healthy subjects using a dual-echo RF-spoiled gradient echo approach at 3T across two institutions. Non-linear registration and tissue density correction were applied.
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