Article
Chemistry, Multidisciplinary
Enrique M. Arpa, Ines Corral
Summary: Unconjugated pterins are widely present and have various enzymatic functions, potentially participating in singlet oxygen, amino acid, and nucleotide photosensitization. Under UV-A light excitation, some of these pterins degrade, leading to hydrogen peroxide production. This process, occurring in vivo, contributes to oxidative stress and melanocyte destruction in vitiligo. Our study provides mechanistic insights into the formation of transient triplet species that trigger Type I and Type II photosensitizing processes and degradation. Through calculations, we demonstrate that 6-biopterin degradation in vitiligo patients' skin produces 6-formylpterin and subsequently 6-carboxypterin. The changes in photosensitizing potential with pH are attributed to modulation of excited-state redox potentials.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Materials Science, Multidisciplinary
Aurash Karimi, Michael Auinger
Summary: This study systematically investigates the diffusion of nitrogen in Ferrite and Austenite using a robust multiscale model combining Density Functional Theory and Kinetic Monte Carlo. Quantitative predictions are made for nitrogen diffusion in vacancy-rich iron crystals, providing valuable insights for nitriding manufacturers. The enhanced diffusion models may play a crucial role in improving existing processes and avoiding common manufacturing problems.
Article
Materials Science, Multidisciplinary
Jakkree Boonlakhorn, Punpatsorn Suksangrat, Jutapol Jumpatam, Weerachai Sarakorn, Sriprajak Krongsuk, Prasit Thongbai, Pornjuk Srepusharawoot
Summary: Na1/2La1/2Cu3Ti4O12 ceramics were successfully synthesized via sol-gel method. The crystal structure of these ceramics is identical to that of CaCu3Ti4O12. CuO and related Cu phases were observed due to the substitution of Na+ at Cu2+ sites. Oxygen vacancies were created during the sintering process, resulting in a lower oxygen vacancy density at room temperature. The sintered Na1/2La1/2Cu3Ti4O12 ceramics exhibited excellent dielectric properties with a high dielectric permittivity and low dielectric loss tangent. Cu+ and Ti3+ observed in the XPS measurements originated from oxygen vacancies in the Na1/2La1/2Cu3Ti4O12 structure. The internal barrier layer capacitor (IBLC) model was found to be the most appropriate for explaining the colossal dielectric response in these ceramics.
MATERIALS CHEMISTRY AND PHYSICS
(2023)
Article
Chemistry, Physical
Oskar Cheong, Michael H. Eikerling, Piotr M. Kowalski
Summary: Classical molecular dynamics simulations were performed to compare water structures with ab initio molecular dynamics simulations. Good agreement was found between the two approaches at the same length and time scales. However, longer trajectories simulated with classical molecular dynamics led to the formation of different, more stable water structures, which were validated with ab initio calculations. This suggests the usefulness and advantage of classical molecular dynamics simulations for sampling more realistic time and length scales in simulations of metal-aqueous solution interfaces.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Physical
Xingdong Gan, Jun Yuan, Haikun Huang, Yanle Li, An Wen, Qiuju Zhang, Chenghua Sun, Baihai Li
Summary: This study proposes using two-dimensional bimetallene as a framework for the lithium metal anode to mitigate the growth of lithium dendrites. Computational investigation shows that bimetallenes with large binding energy and low diffusion barrier are beneficial for the uniform deposition of lithium. Experimental results demonstrate that AgMn bimetallene has the capability to suppress lithium dendrites.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Xun-Jian Hu, Yi Yang, Chunju Hou, Tong-Xiang Liang
Summary: Perovskite oxides are versatile materials with rich properties, and recent research has shown that freestanding two-dimensional structures down to the monolayer limit can be prepared. The study reveals that 2D perovskite oxides exhibit abnormal band-gap trends, with a gap value lower than the bulk limit, indicating the presence of an unusual quantum size effect. The electronic properties of 2D perovskite oxides evolve with dimension change, with termination-dependent thermodynamic stability and band splitting contributing to the abnormal trends.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Shuo Cao, Gang Zhao, Dehua Wang
Summary: Using fully ab initio molecular dynamics simulations, this study investigates the inherent structure of water and its temperature dependence. The results reveal three types of translational ordering in the second oxygen coordination shell, leading to the classification of local structures in water into three types. These findings provide ab initio evidence for the mixture model of water and shed light on the temperature dependence of its inherent structure.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Abdelazim M. Mebed, Muhammad Mushtaq, Muhammad Faizan, Riadh Neffati, Amel Laref, Sumegha Godara, Sana Maqbool
Summary: In this study, the adsorption of CO molecule on the (001) surface of Heusler alloy CrCoIrGa was investigated using DFT+U calculations. It was found that the surface retained the bulk atomic positions with no surface reconstruction, but had more spin-polarization and atomic moments due to the presence of unsaturated bonds. The most favorable adsorption configuration was found to be with the CO molecule adsorbed on the top of the Ir atom. This indicates a strong interaction (chemisorption) between the (001) surface and CO gas molecule, suggesting potential applications in gas sensing.
Article
Chemistry, Physical
Sahbi Trabelsi, Mouadh Tlili, Hafedh Abdelmoulahi, Salah Bouazizi, Salah Nasr, Miguel A. Gonzalez, Marie-Claire Bellissent-Funel, Jacques Darpentigny
Summary: A detailed analysis of the equimolar methanol-water (MeW) liquid structure at 298 K and atmospheric pressure was performed using neutron scattering, Density Functional Theory (DFT) calculation, and Molecular Dynamics (MD) simulations. The results showed the formation of water-methanol H-bonded clusters in the MeW mixture, leading to a decrease in the self-diffusion coefficients of the monomers.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Chemistry, Physical
Joseph P. Heindel, Sotiris S. Xantheas
Summary: A protocol for classical and nuclear quantum dynamics is presented, utilizing the many-body expansion (MBE) for generating energies and forces, applied to water clusters using different interaction potentials at various temperatures. Results show that a four-body description of energies and forces is essential for accurate anharmonic vibrational frequencies.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Article
Chemistry, Multidisciplinary
Loic Groslambert, Yann Cornaton, Matej Ditte, Emmanuel Aubert, Patrick Pale, Alexandre Tkatchenko, Jean-Pierre Djukic, Victor Mamane
Summary: Telluronium salts [Ar2MeTe]X were synthesized and their Lewis acidic properties in solution were investigated using physical and theoretical methods. The study revealed the electrophilicity of the Te centers and the ability of telluroniums to form Lewis pairs. The affinity of telluroniums for OPPh3 was determined by state-of-the-art computational methods, showing the importance of Coulombic and dispersion interactions in solution.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Ruinian Xu, Ning Liu, Chengna Dai, Yan Li, Jie Zhang, Bin Wu, Gangqiang Yu, Biaohua Chen
Summary: By introducing H2O molecules on Cu-BEA zeolites, the selectivity, productivity, and long-term stability of direct oxidation of methane to methanol can be significantly improved.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Crystallography
J. M. Ramirez-de-Arellano, A. Fransuani Jimenez G., L. F. Magana
Summary: The study found that doping a hexagonal boron nitride surface with Ti or Pt can influence the adsorption of CO2 molecules in different ways. Titanium atoms allow for the chemisorption of CO2 molecules, while platinum atoms result in the repulsion of CO2 molecules.
Article
Materials Science, Multidisciplinary
Kirill N. Boldyrev, Vadim S. Sedov, Danny E. P. Vanpoucke, Victor G. Ralchenko, Boris N. Mavrin
Summary: The vibrational behavior of the germanium-vacancy (GeV) in diamond has been studied using photoluminescence spectrum and first-principles modeling. Two localized modes associated with the GeV center and neighboring carbon atoms have been identified, corresponding to the observed features in the photoluminescence spectrum.
DIAMOND AND RELATED MATERIALS
(2022)
Article
Nanoscience & Nanotechnology
B. Akdim, C. Woodward, S. Rao, E. Antillon
Summary: Recent studies have shown that chemically-complex solid-solution alloys produce equilibrium dislocations at high temperatures, leading to kinks and pinning points that significantly increase strength. Atomistic studies and chemical analysis can help understand the effects of different alloy compositions on dislocation formation.
SCRIPTA MATERIALIA
(2021)
Article
Chemistry, Physical
Giampaolo Ricciardi, Evert Jan Baerends, Angela Rosa
Letter
Chemistry, Physical
Evert Jan Baerends, Oleg Gritsenko
JOURNAL OF CHEMICAL PHYSICS
(2016)
Article
Chemistry, Physical
R. van Meer, O. V. Gritsenko, E. J. Baerends
JOURNAL OF CHEMICAL PHYSICS
(2017)
Article
Chemistry, Physical
E. J. Baerends
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2017)
Article
Chemistry, Physical
Leonardo Bernasconi, Andranik Kazaryan, Paola Belanzoni, Evert Jan Baerends
Article
Physics, Condensed Matter
Paola Gori-Giorgi, Evert Jan Baerends
EUROPEAN PHYSICAL JOURNAL B
(2018)
Article
Chemistry, Physical
R. van Meer, O. V. Gritsenko, E. J. Baerends
JOURNAL OF CHEMICAL PHYSICS
(2018)
Article
Chemistry, Physical
Evert Jan Baerends
JOURNAL OF CHEMICAL PHYSICS
(2018)
Article
Chemistry, Physical
E. J. Baerends
Article
Chemistry, Physical
M. Amati, S. Stoia, E. J. Baerends
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2020)
Article
Chemistry, Inorganic & Nuclear
Mario Amati, Evert Jan Baerends, Giampaolo Ricciardi, Angela Rosa
INORGANIC CHEMISTRY
(2020)
Article
Physics, Multidisciplinary
Jian Wang, Evert Jan Baerends
Summary: A self-consistent field method based on density matrix functional theory is proposed, which reduces the computational cost while maintaining the accuracy compared to sophisticated configuration interaction based methods. This method effectively includes both weak or breaking bond nondynamical correlation and dynamical correlation at all distances in a single scheme. It is well suited for large-scale potential energy surface calculation and molecular dynamics simulation.
PHYSICAL REVIEW LETTERS
(2022)
Article
Chemistry, Physical
Sara Giarrusso, Roeland Neugarten, Evert Jan Baerends, Klaas J. H. Giesbertz
Summary: In this study, we consider a prototypical 1D model Hamiltonian for a stretched heteronuclear molecule and investigate the characteristics of its individual components. We find that these components exhibit peaks and steps in regions with very low density. By analyzing an analytical model, we explain the underlying mechanism behind these characteristics and evaluate the validity of the model at large but finite internuclear distance.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Physical
Andrew M. Teale, Trygve Helgaker, Andreas Savin, Carlo Adamo, Balint Aradi, Alexei Arbuznikov, Paul W. Ayers, Evert Jan Baerends, Vincenzo Barone, Patrizia Calaminici, Eric Cances, Emily A. Carter, Pratim Kumar Chattaraj, Henry Chermette, Ilaria Ciofini, T. Daniel Crawford, Frank De Proft, John F. Dobson, Claudia Draxl, Thomas Frauenheim, Emmanuel Fromager, Patricio Fuentealba, Laura Gagliardi, Giulia Galli, Jiali Gao, Paul Geerlings, Nikitas Gidopoulos, Peter M. W. Gill, Paola Gori-Giorgi, Andreas Gorling, Tim Gould, Stefan Grimme, Oleg Gritsenko, Hans Jorgen Aagaard Jensen, Erin R. Johnson, Robert O. Jones, Martin Kaupp, Andreas M. Koster, Leeor Kronik, Anna Krylov, Simen Kvaal, Andre Laestadius, Mel Levy, Mathieu Lewin, Shubin Liu, Pierre-Francois Loos, Neepa T. Maitra, Frank Neese, John P. Perdew, Katarzyna Pernal, Pascal Pernot, Piotr Piecuch, Elisa Rebolini, Lucia Reining, Pina Romaniello, Adrienn Ruzsinszky, Dennis R. Salahub, Matthias Scheffler, Peter Schwerdtfeger, Viktor N. Staroverov, Jianwei Sun, Erik Tellgren, David J. Tozer, Samuel B. Trickey, Carsten A. Ullrich, Alberto Vela, Giovanni Vignale, Tomasz A. Wesolowski, Xin Xu, Weitao Yang
Summary: This paper provides an informal review and discussion on the history, present status, and future of density-functional theory (DFT) by 70 workers in the field. The format of a roundtable discussion allowed participants to express their views through 302 individual contributions to a preset list of 26 questions. Supported by a bibliography of 777 entries, the paper offers a comprehensive snapshot of DFT in 2022.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
E. J. Baerends
Summary: The translated article discusses the concept of the chemical potential of electrons in an atom or molecule in the density functional theory. It points out that the chemical potential cannot be defined in few-electron systems because they lack important characteristics of thermodynamic systems. The article also critically reviews some issues in density functional theory.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)