Article
Multidisciplinary Sciences
You Meng, Xiaocui Li, Xiaolin Kang, Wanpeng Li, Wei Wang, Zhengxun Lai, Weijun Wang, Quan Quan, Xiuming Bu, SenPo Yip, Pengshan Xie, Dong Chen, Dengji Li, Fei Wang, Chi-Fung Yeung, Changyong Lan, Chuntai Liu, Lifan Shen, Yang Lu, Furong Chen, Chun-Yuen Wong, Johnny C. Ho
Summary: The authors explore the unique multi-scale van der Waals interactions in one-dimensional tellurium systems to overcome the restrictions imposed by chemical bonds. They succeed in synthesizing wafer-scale van der Waals nanomeshes composed of self-welding Te nanowires on various substrates at a low temperature, which exhibit improved transport and photoelectric properties. These Te vdWs nanomesh electronics hold great promise in meeting emerging technological demands.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Shota Ono, Junji Yuhara, Jun Onoe
Summary: The study shows that although lead and tin are immiscible, they can form alloys on the surfaces of other metals. By analyzing the stability of ordered alloys PbZ and SnZ in different structures, the phenomena observed in previous experiments can be explained.
CHEMICAL PHYSICS LETTERS
(2021)
Article
Chemistry, Physical
Logan J. Augustine, Ali Abbaspour Tamijani, Jennifer L. Bjorklund, Hind A. Al-Abadleh, Sara E. Mason
Summary: The interactions between organic molecules and mineral surfaces are influenced by various factors, including adsorbate speciation, surface atomic and electronic structure, and environmental conditions. This study used Density Functional Theory (DFT) to model the inner-sphere adsorption of oxalate and pyrocatechol on different alpha-Fe2O3 surfaces. The results revealed that each surface facet has a unique factor that determines the site preference. The findings provide insights into understanding the adsorption processes occurring at the surface-aqueous interface.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Article
Biochemistry & Molecular Biology
Xiaoji Zhao, Yanlu Li, Xian Zhao
Summary: This study investigates the structure, stability, and electronic structure of hydrogen and oxygen vacancy defects on the (100) and (101) growth surfaces of KDP crystals using density functional theory. The effects of acidic and alkaline environments on surface defects are also discussed. The results show that different vacancy defects have varying properties on different surfaces, and acidic environments are conducive to repairing surface defects.
Article
Chemistry, Physical
Ningjing Luo, Zhufeng Hou, Guo-Liang Chai
Summary: This study systematically explores the catalytic activity of tungsten monocarbide (WC) by studying the methane dehydrogenation and C-C coupling processes on WC surfaces using density functional theory (DFT) calculations. The results indicate that the W-terminated WC(0001) surface is the most favorable exposed surface with a lower surface energy. Additionally, the Co(111), Ni(111), and W-terminated WC(0001) surfaces exhibit similar catalytic properties in methane dehydrogenation, and the rate-limiting step on the W-terminated WC(0001) surface is the dissociation of CH*. C-C coupling through CH* intermediates on the W-terminated WC(0001) surface favors the formation of C2H2 kinetically.
APPLIED SURFACE SCIENCE
(2022)
Review
Materials Science, Multidisciplinary
Hairui Xing, Ping Hu, Shilei Li, Yegai Zuo, Jiayu Han, Xingjiang Hua, Kuaishe Wang, Fan Yang, Pengfa Feng, Tian Chang
Summary: First-principle calculations, particularly using density functional theory (DFT), are employed to investigate the structure and properties of oxygen/metal interfaces, specifically focusing on the adsorption and diffusion behavior of oxygen molecules or atoms on metal surfaces. This review aims to contribute to the understanding of adsorption properties and diffusion behavior on a metal surface at an atomic-scale, particularly for those interested in catalytic oxidation and corrosion applications.
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
(2021)
Review
Materials Science, Coatings & Films
Raymond T. Tung
Summary: For many decades, the mystery surrounding the formation mechanism of the Schottky barrier height (SBH) was dominated by the concept of Fermi-level pinning (FLP). However, experimental research on polycrystalline metal-semiconductor interfaces revealed insensitivity of the SBH to metal work function, leading to a shift in understanding and the proposal of new theories.
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A
(2021)
Article
Physics, Multidisciplinary
Tomasz Maciazek
Summary: The reduced density matrix functional theory is a powerful tool for studying properties of ground states of strongly interacting quantum many body systems, especially Bose-Einstein condensation and systems of strongly correlated electrons. It has been shown that the density functional in these systems exhibits a repulsive gradient, known as the Bose-Einstein condensation force, which is universal for different types of pair-interaction and non-homogeneous gases. The theory has also been extended to fermionic systems, showing the existence of a similar repulsive gradient in the fermionic RDMFT.
NEW JOURNAL OF PHYSICS
(2021)
Article
Materials Science, Multidisciplinary
Radek Jesko, Ondrej Stejskal, Robin Silber, Lukas Beran, Martin Veis, Ahmad Omar, Jaroslav Hamrle
Summary: The study analyzed the optical and magneto-optical properties of the Heusler compound Co2FeAl0.5Si0.5, showing that the spectral permittivity is mainly influenced by absorption by minority electrons. The best agreement between experimental and theoretical results was found for the local density approximation potential, with the half-metallic ferromagnetic character preserved only in calculations using the Coulomb interaction correction.
Article
Chemistry, Physical
Aaron D. Kaplan, Stewart J. Clark, Kieron Burke, John P. Perdew
Summary: Classical turning surfaces of Kohn-Sham potentials separate classically allowed regions (CARs) from classically forbidden regions (CFRs). The presence and distribution of CFRs vary in different materials based on factors such as material type and internuclear distances. Many semiconductors have no CFR at equilibrium, which is crucial for density functional construction.
NPJ COMPUTATIONAL MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Shujie Zhang, Kejiang Li, Yan Ma, Yushan Bu, Zeng Liang, Zonghao Yang, Jianliang Zhang
Summary: This study employs density functional theory (DFT) to investigate the adsorption behavior of hydrogen atoms and H-2 on different crystal FeO surfaces. It reveals that Fe (catalytic site) and O (binding site) atoms contribute to the interaction between H-2 and FeO surfaces.
Article
Materials Science, Multidisciplinary
Jia-Li Chen, Nikolas Kaltsoyannis
Summary: Understanding actinide mixed oxides is crucial for the development of nuclear fuel and the storage of spent fuel. This study provides systematic simulations of AnO(2) and U-An MOX using density functional theory, focusing on spin density and density of states. Conclusions are drawn regarding oxidation states and transition regions between different systems.
JOURNAL OF NUCLEAR MATERIALS
(2022)
Article
Chemistry, Physical
Hui Zhang, Qi-Chao Liu, Chun-Qi Zhou, Zi-Hao Yue, Zhen-Kun Tang
Summary: Novel 2D functionalized hexagonal boron phosphides breaking mirror symmetry are demonstrated as potential high efficiency water splitting photocatalysts. These catalysts exhibit moderate band gap, spatial separation of photoexcited carriers, and strong light absorption.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Laura von Lueders, Rita Tilmann, Kangho Lee, Cian Bartlam, Tanja Stimpel-Lindner, Tarja K. Nevanen, Kristiina Iljin, Kathrin C. Knirsch, Andreas Hirsch, Georg S. Duesberg
Summary: We present a controllable and specific functionalisation approach for graphene field-effect transistors (GFETs) in order to detect small physiologically active molecules. The key step involves the noncovalent functionalisation of graphene with perylene bisimide (PBI) molecules directly on the growth substrate. This method allows for the homogeneous self-assembly of PBI molecules on graphene, followed by the immobilization of antibodies. The functionalised GFET devices showed excellent performance in terms of atomic force microscopy, Raman spectroscopy, and electrical measurements compared to conventional functionalisation methods. Specific sensing of small molecules such as methamphetamine and cortisol was achieved by monitoring the electrical changes of the functionalised GFET devices. The sensors were able to detect methamphetamine down to a concentration of 300 ng ml(-1).
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Keita Kobayashi, Akiko Yamaguchi, Masahiko Okumura
Summary: Machine learning molecular dynamics (MLMD) is a promising method for accurately predicting material properties with low computational costs. By utilizing machine learning potentials (MLPs), the structural and mechanical properties of materials can be evaluated and compared with other simulations and experimental results.
APPLIED CLAY SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Yonggui Zhao, Nanchen Dongfang, Carlos A. Triana, Chong Huang, Rolf Erni, Wenchao Wan, Jingguo Li, Dragos Stoian, Long Pan, Ping Zhang, Jinggang Lan, Marcella Iannuzzi, Greta R. Patzke
Summary: The rational design of efficient electrocatalysts for industrial water splitting is crucial for sustainable hydrogen fuel generation. In this study, hierarchically nanostructured Co@CoFe-P NBs were introduced as alternative electrocatalysts for industrial-scale applications. Operando analysis and theoretical calculations revealed the catalytic mechanisms of these electrocatalysts in hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), providing important insights for future energy conversion and storage.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Article
Physics, Condensed Matter
Michela Pauletti, Vladimir V. Rybkin, Marcella Iannuzzi
Summary: In this work, we assess and extend strategies for calculating surface tension of complex liquids from molecular dynamics simulations, including the mechanical route and the ILI approach. We generalize the ILI method to complex molecular liquids using atomic van der Waals radii. The performance of these approaches is evaluated on acetonitrile and water-methanol mixture, and the effect of different computational models on the estimate of surface tension is compared.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2022)
Article
Multidisciplinary Sciences
Hirofumi Yanagisawa, Markus Bohn, Florian Goschin, Ari P. Seitsonen, Matthias F. Kling
Summary: By applying strong direct current electric fields on a sharp metallic tip, electrons can be emitted radially from the apex to vacuum, magnifying nanoscopic information on the apex and creating a field emission microscope (FEM). This study used fullerene molecules to characterize the molecule-covered tip through experiments and simulations. The results suggest that the peculiar electron emission patterns originate from a molecule layer formed on the tip under strong DC electric fields.
SCIENTIFIC REPORTS
(2022)
Article
Geochemistry & Geophysics
Gleb S. Pokrovski, Elsa Desmaele, Clement Laskar, Elena F. Bazarkina, Denis Testemale, Jean-Louis Hazemann, Rodolphe Vuilleumier, Ari Paavo Seitsonen, Guillaume Ferlat, Antonino Marco Saitta
Summary: Gold mobilization, transfer, and concentration in the Earth's crust are controlled by hydrothermal sulfur- and chloride-bearing fluids. The exact chemical identity, structure, and stability of Au-bearing species and the respective contributions of the sulfide and trisulfur ion ligands to Au transport lack direct evidence. In this study, high energy resolution fluorescence detection X-ray absorption spectroscopy (HERFD-XAS) was used to investigate solutions containing sulfate, sulfide, and S-3(center dot-). The results showed differences in dissolved Au spectral signatures indicative of contrasting fluid-phase Au speciation as a function of acidity and redox conditions. The spectroscopic data, combined with other measurements and models, confirmed the existence of Au(HS)S-3(-), Au(HS)(2)(-), and Au(HS)(3)- complexes under different conditions. These findings provide direct evidence for the speciation of Au in aqueous S-bearing fluids and highlight the importance of the trisulfur ion in gold mobilization and concentration.
AMERICAN MINERALOGIST
(2022)
Article
Materials Science, Multidisciplinary
Johannes T. Kuechle, Aleksandr Baklanov, Ari P. Seitsonen, Paul T. P. Ryan, Peter Feulner, Prashanth Pendem, Tien-Lin Lee, Matthias Muntwiler, Martin Schwarz, Felix Haag, Johannes Barth, Willi Auwaerter, David A. Duncan, Francesco Allegretti
Summary: This research reveals the presence of a second silicon species, a Si-Ag alloy, between the silicene and the silver substrate, which provides support for the silicene layer. The findings challenge the current understanding of the structural properties of the silicene/Ag(111) interface and may have implications for the stabilization of other 2D materials grown epitaxially on metal surfaces.
Article
Chemistry, Multidisciplinary
Peter Knecht, Dennis Meier, Joachim Reichert, David A. Duncan, Martin Schwarz, Johannes T. Kuechle, Tien-Lin Lee, Peter S. Deimel, Peter Feulner, Francesco Allegretti, Willi Auwaerter, Guillaume Medard, Ari Paavo Seitsonen, Johannes Barth, Anthoula C. Papageorgiou
Summary: Ru-porphyrins serve as pedestals for the assembly of N-heterocyclic carbenes (NHCs) on solid surfaces. A phenomenon of transferring Ru-porphyrin molecules from the surface to the next layer can be observed upon deposition of a simple NHC ligand on a close-packed Ru-porphyrin monolayer. The uptake of NHC induces a rearrangement of the molecular layer, which can be reversed by thermal desorption of the NHC ligand. Understanding such mass transport processes is crucial for surface functionalization with carbenes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Beliz Sertcan, Seyyed Jabbar Mousavi, Marcella Iannuzzi, Peter Hamm
Summary: Theoretical calculations of low-frequency anharmonic couplings in the beta-phase of crystalline bromoform were conducted based on density functional theory quantum chemistry calculations. The dominant role of electrical anharmonicity in the 2D Raman-THz response of both crystalline and liquid bromoform was revealed. The difference in relative cross-peak intensities between intramolecular and intermolecular modes in bromoform can be explained by the C-3v symmetry of bromoform along with orientational averaging.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
T. Demchuk, T. Bryk, A. P. Seitsonen
Summary: We conducted an ab initio simulation study on liquid Si at pressures ranging from 10.2 to 24.3 GPa along the isothermal line of 1150 K. Increasing the pressure from 10.2 to 16 GPa led to a significant decrease in the tetrahedral ordering of the closest neighbors. The diffusion coefficient exhibited a linear decay with a drop in atomic volume, in agreement with theoretical predictions for simple liquid metals.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Physics, Condensed Matter
T. Bryk, I-m Ilenkov, A. P. Seitsonen
Summary: We performed ab initio simulation and theoretical study on collective dynamics in liquid Sb at 973 K. By applying the GCM theoretical approach to analysis of simulation-derived time correlation functions, we identified two types of propagating eigenmodes. We found that the flat dispersion of the high-frequency branch of propagating modes can be explained by out-of-phase oscillations of nearest neighbors forming quasi-bound atomic pairs for at least 30 ps. We discussed the collective dynamics features in non-simple metallic melts containing quasi-bound pairs.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2023)
Article
Chemistry, Physical
Augustin Bussy, Ole Schutt, Jurg Hutter
Summary: The development of novel double-hybrid density functionals has led to higher levels of accuracy and insights into matter's fundamental properties. Low-scaling methods for Hartree-Fock exchange, SOS-MP2, and direct RPA energy gradients have been developed and implemented in the CP2K software package, enabling their application to large and periodic systems.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Fabian Belleflamme, Anna-Sophia Hehn, Marcella Iannuzzi, Juerg Hutter
Summary: Accurate descriptions of intermolecular interactions are crucial for molecular liquid simulations. To achieve both accuracy and computational efficiency, we propose an electronic structure method that combines the Harris functional approach with approximately linear-scaling density functional theory (DFT). By constructing a Lagrangian energy functional, the non-variational nature of the Harris functional is addressed. The method allows for simulations with accuracies close to the Kohn-Sham DFT reference, making it suitable for ab initio molecular dynamics simulations of large molecular systems.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Physics, Condensed Matter
R. Vuilleumier, A. P. Seitsonen
Summary: In this study, we investigated the vibrations of water using molecular dynamics simulations, focusing on Raman and infrared spectroscopic signatures. We analyzed the effects of temperature on the vibrational frequencies and examined the role of hydrogen bonding coordination by using restrained simulations. Additionally, we compared the impacts of different methods of solving the electronic structure on evaluating ion forces and reported results on angular correlations, isotopic mixtures, and dielectric constants in water.
CONDENSED MATTER PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Fernand E. E. Torres-Davila, Chance Barrett, Michael Molinari, Muhammad Sajid, Ari P. P. Seitsonen, Abdelkader Kara, Laurene Tetard
Summary: Defect engineering in two-dimensional materials has expanded their applications in catalysis, nanoelectronics, sensing, and more. Due to limited tools for exploring nanoscale functional properties in non-vacuum environments, theoretical modeling provides valuable insights into the effects of local deformations on experimental signals obtained by nanoscale chemical imaging. By using atomic force microscopy and infrared light under an inert environment, we demonstrate the controlled creation of nanoscale strained defects in hexagonal boron nitride (h-BN). Nanoscale IR spectroscopy reveals the broadening of the in-plane phonon (E-1u) mode of h-BN during defect formation, while density functional theory-based calculations and molecular dynamics quantify the tensile and compressive strain in the deformation.
Article
Chemistry, Physical
Giacomo Melani, Juan Pablo Guerrero-Felipe, Ana M. Valencia, Jannis Krumland, Caterina Cocchi, Marcella Iannuzzi
Summary: In this study, the structural, energetic, and electronic properties of molecular donors and acceptors adsorbed on hBN and MoS2 monolayers were investigated using density-functional theory. The stability of all interfaces was found to be due to dispersion interactions and the flat arrangement of molecules. Level alignment on hBN depended on the frontier orbitals' energies, forming either type-I or type-II interfaces, while all MoS2-based systems exhibited type-II alignment. Interfacial dipole moments and wave-function hybridization further influenced the electronic structure of the hybrid materials, providing important insights for designing novel low-dimensional materials for opto-electronics.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
