In Paper I of this series [F. A. Bischoff, "Regularizing the molecular potential in electronic structure calculations. I. SCF methods," J. Chem. Phys. 141, 184105 (2014)] a regularized molecular Hamilton operator for electronic structure calculations was derived and its properties in SCF calculations were studied. The regularization was achieved using a correlation factor that models the electron-nuclear cusp. In the present study we extend the regularization to correlated methods, in particular the exact solution of the two-electron problem, as well as second-order many body perturbation theory. The nuclear and electronic correlation factors lead to computations with a smaller memory footprint because the singularities are removed from the working equations, which allows coarser grid resolution while maintaining the precision. Numerical examples are given.
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http://dx.doi.org/10.1063/1.4901022 | DOI Listing |
Angew Chem Int Ed Engl
January 2025
University of Electronic Science and Technology of China, State Key Laboratory of Electronic Thin Films and Integrated Devices, No. 2006, Xiyuan Avenue, High-tech Zone (West Area), 610054, Chengdu, CHINA.
Bismuth oxide (Bi2O3) emerges as a potent catalyst for converting CO2 to formic acid (HCOOH), leveraging its abundant lattice oxygen and the high activity of its Bi-O bonds. Yet, its durability is usually impeded by the loss of lattice oxygen causing structure alteration and destabilized active bonds. Herein, we report an innovative approach via the interstitial incorporation of indium (In) into the Bi2O3, significantly enhancing bond stability and preserving lattice oxygen.
View Article and Find Full Text PDFACS Mater Au
January 2025
Department of Electronic Systems Engineering, Indian Institute of Science, Bangalore 560012, India.
The delivery of molecules, such as DNA, RNA, peptides, and certain hydrophilic drugs, across the epidermal barrier poses a significant obstacle. Microneedle technology has emerged as a prominent area of focus in biomedical research because of its ability to deliver a wide range of biomolecules, vaccines, medicines, and other substances through the skin. Microneedles (MNs) form microchannels by disrupting the skin's structure, which compromises its barrier function, and facilitating the easy penetration of drugs into the skin.
View Article and Find Full Text PDFNanoscale
January 2025
Photon Science Research Center for Carbon Dioxide, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China.
Oxygen vacancies (V's) are of paramount importance in influencing the properties and applications of ceria (CeO). Yet, comprehending the distribution and nature of V's poses a significant challenge due to the vast number of electronic configurations and intricate many-body interactions among V's and polarons (Ce ions). In this study, we established a cluster expansion model based on first-principles calculations and statistical learning to decouple the interactions among the Ce ions and V's, thereby circumventing the limitations associated with sampling electronic configurations.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
Faculty of Chemistry, University of Gdańsk, Wita Stwosza 63, 80-308 Gdańsk, Poland.
Carbonless DNA was designed by replacing all carbon atoms in the standard DNA building blocks with boron and nitrogen, ensuring isoelectronicity. Electronic structure quantum chemistry methods (DFT(ωB97XD)/aug-cc-pVDZ) were employed to study both the individual building blocks and the larger carbon-free DNA fragments. The reliability of the results was validated by comparing selected structures and binding energies using more accurate methods such as MP2, CCSD, and SAPT2+3(CCD)δ.
View Article and Find Full Text PDFInorg Chem
January 2025
Research Institute for Electronic Science, Hokkaido University, Sapporo 001-0021, Japan.
Electrochemical devices that can operate at temperatures of 200-300 °C are expected to become the next-generation energy conversion devices in fuel cells and electrosynthesis, which are important for achieving carbon neutrality. Proton conductors based on phosphate glasses are being developed as candidate materials for such devices. We recently developed a glass proton conductor by using silicophosphoric acid based on the idea of solidifying phosphoric acid with silicon as a cross-linking glass framework.
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