Article
Materials Science, Multidisciplinary
Niels Ehlen, Yannic Falke, Boris V. Senkovskiy, Timo Knispel, Jeison Fischer, Oliver N. Gallego, Cesare Tresca, Maximilian Buchta, Konstantin P. Shchukin, Alessandro D'Elia, Giovanni Di Santo, Luca Petaccia, Dmitry Smirnov, Anna Makarova, Gianni Profeta, Thomas Michely, Alexander Grueneis
Summary: This study demonstrates the orbital-selectivity of Fe doping in epitaxial MoS2 using angle-resolved photoemission spectroscopy (ARPES) and further validates it through other experiments and calculations. The results show that dopants with complex d-orbital structure interact with MoS2 bands in an orbital-sensitive manner.
Article
Thermodynamics
Yuxiang Zhu, Chong-Wen Zhou, Alexander A. Konnov
Summary: In this study, the reaction kinetics of hydrogen-abstraction reactions from methoxymethanol by various radicals were investigated using high-level ab initio calculations. It was found that the H-abstraction reactions from the secondary carbon atom of methoxymethanol are favored pathways. Different radicals have different rate constants for hydrogen-abstraction reactions at different temperatures.
COMBUSTION AND FLAME
(2021)
Article
Chemistry, Physical
Soulef Jellali, Hela Habli
Summary: This paper focuses on the study of molecules such as francium dimer and a comparative spectroscopic investigation of cationic systems Fr-(Ca+, Sr+, Ba+). Computational methods are used to determine relevant parameters and the accuracy and reliability of the results are discussed. The findings provide insights for future laser cooling applications.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Physical
Juan J. J. Aucar, Alejandro F. F. Maldonado, Juan I. I. Melo
Summary: In this work, relativistic corrections to the electric field gradient (EFG) are presented, including spin-dependent corrections for the first time. The results show that these new corrections significantly improve the performance of the existing method and are in close agreement with calculations at the four-component Dirac-Hartree-Fock (4c-DHF) level. The accuracy of the EFG values obtained with this new method allows for the analysis of the electronic origin of relativistic effects using well-known nonrelativistic operators.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Materials Science, Coatings & Films
Petr Rehak, Jakub Ceska, Miroslav Cerny
Summary: Using a first-principles approach, the effect of oxygen as a substitutional impurity on the cohesion of three transition metal nitride multilayers was investigated. It was found that oxygen prefers to replace nitrogen atoms in interfacial planes and does not reduce the multilayer cohesion. In fact, in the AlN/TiN system, the presence of oxygen was found to increase the cohesion of the interface.
SURFACE & COATINGS TECHNOLOGY
(2023)
Article
Materials Science, Multidisciplinary
Keisuke Mukai, Ryuta Kasada, Jae-Hwan Kim, Masaru Nakamichi
Summary: In this study, first-principles calculations were performed on 42 existing binary Be intermetallics to find an effective electronic descriptor. The occupied Be p band center relative to the Fermi level was identified as a bulk descriptor, correlating with the Be vacancy formation energy. The bulk descriptor was confirmed to be an experimentally measurable scale, which can accelerate the material development of beryllium intermetallic neutron multipliers.
Article
Chemistry, Physical
Jing Shang, Congxin Xia, Chun Tang, Chun Li, Yandong Ma, Yuantong Gu, Liangzhi Kou
Summary: The bending deformation of AgBiP2Se6 monolayers can manipulate the polarization direction and domain size, significantly improving the ferroelectric stability. This mechano-ferroelectric coupling represents a new mechanism for stabilization and polarization flip in 2D ferroelectrics, with potential applications in next-generation non-volatile storage devices.
NANOSCALE HORIZONS
(2021)
Article
Chemistry, Multidisciplinary
Dumitru-Claudiu Sergentu, Corwin H. Booth, Jochen Autschbach
Summary: The Ce L-3 edge XAS spectra of CeO2 and cerocene were accurately calculated using relativistic ab-initio multireference wavefunction approaches. The study aimed to solve the puzzle regarding the relationship between the XAS peaks and the 4f electron occupation. The calculated GS 4f-shell occupations show good agreement with measurements, indicating Ce IV and III oxidation numbers.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Editorial Material
Chemistry, Multidisciplinary
Dumitru-Claudiu Sergentu, Corwin H. Booth, Jochen Autschbach
Summary: The Ce L-3 edge XAS spectra of CeO2 and cerocene were calculated using relativistic ab-initio multireference wavefunction approaches to accurately reproduce observed spectra. The study aimed to resolve the long-standing puzzle regarding the relationship between XAS peaks and 4f electron occupation in ground state versus core-excited states. The roles of covalent bonding and wavefunction configurational composition in intensity patterns were highlighted, along with the agreement between calculated GS 4f-shell occupations and XAS measurements using peak areas.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Peter Knecht, Joachim Reichert, Peter S. Deimel, Peter Feulner, Felix Haag, Francesco Allegretti, Manuela Garnica, Martin Schwarz, Willi Auwaerter, Paul T. P. Ryan, Tien-Lin Lee, David A. Duncan, Ari Paavo Seitsonen, Johannes V. Barth, Anthoula C. Papageorgiou
Summary: This study investigates the binding of CO to Ru-porphyrins on an Ag(111) substrate, demonstrating that substituents can regulate the interfacial conformational adaptability, either promoting or obstructing the uptake of axial CO adducts. The research combines real-space visualization, manipulation experiments, and density-functional-theory calculations to provide insights into the functional interface.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Biochemistry & Molecular Biology
Fedor Y. Naumkin
Summary: Complexes of metal atoms with organic molecules are a class of systems with numerous applications, such as in metal-organic interfaces and organometallic chemistry. This study systematically investigates complexes with second-group metals, focusing on their structure, stability, charge distribution, polarity, and IR spectra. Three groups of isomers with different stability and physisorption or chemisorption characteristics are identified. Nonadditive stabilization in ternary systems and shape alterations of the aromatic component for different isomers and system sizes are also observed.
Article
Nanoscience & Nanotechnology
Fatima Akhtar, Jaroslaw Dabrowski, Rasuole Lukose, Christian Wenger, Mindaugas Lukosius
Summary: This study demonstrates the importance of uniform growth in the fabrication of graphene devices by reporting on the growth of large-scale, high-quality monolayer graphene on semiconducting 8-inch Ge(110)/Si wafers using chemical vapor deposition. The quality of graphene is indicated by small FWHM of the Raman 2D band, low intensity ratio of the Raman D and G bands, and homogeneous SEM images. Hall measurements confirm the high mobility and low sheet resistance of the graphene. The difference in growth mechanisms between Ge(001) and Ge(110) is attributed to their unique surface geometries and complex reconstructions.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Nanoscience & Nanotechnology
Puspamitra Panigrahi, Yash Pal, Thanayut Kaewmaraya, Hyeonhu Bae, Noushin Nasiri, Tanveer Hussain
Summary: There is a growing demand for fast, reliable, inexpensive, non-invasive, sensitive, and compact sensors in various fields. Efficient detection of chemical warfare agents is of great importance, and molybdenum carbide MXenes have been explored as efficient sensors for selected chemical warfare agents. Calculations based on density functional theory revealed strong chemisorption of CWAs with Mo2CF2 and Mo2CS2 monolayers, while Mo2CO2 exhibited comparatively weak bindings. The variations in electronic properties and work functions upon CWA adsorption authenticate the efficient sensing mechanism. Statistical thermodynamic analysis was applied to explore the sensing properties of Mo2CTx at different temperatures and pressures, paving the way for low-cost reusable sensors for CWA detection.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Physical
Filipe Menezes, Grzegorz Maria Popowicz
Summary: This study calculates the Gibbs energies for a network of reactions related to the hydrolysis of nitrogen dioxide (NO2) using high-level quantum chemistry. With solvation corrections, temperature dependent thermodynamic data in liquid water are determined. The results show that nitrogen dioxide can be fully converted to nitric and nitrous acid under certain conditions. This research has significant potential impact on the understanding of atmospheric chemistry and the reduction of anthropomorphic pollution.
Article
Multidisciplinary Sciences
M. Tyunina, O. Pacherova, T. Kocourek, A. Dejneka
Summary: The study demonstrates that oxygen vacancies in ABO(3) perovskite oxides primarily result in strong anisotropic strain in epitaxial thin films, rather than weak isotropic expansion in bulk samples. This anisotropic chemical strain is explained by the preferential orientation of elastic dipoles of the vacancies, which have critical impacts on the synthesis and response functions of the films.
SCIENTIFIC REPORTS
(2021)
Review
Physics, Condensed Matter
Boeri Lilia, Richard Hennig, Peter Hirschfeld, Gianni Profeta, Antonio Sanna, Eva Zurek, Warren E. Pickett, Maximilian Amsler, Ranga Dias, Mikhail Eremets, Christoph Heil, Russell J. Hemley, Hanyu Liu, Yanming Ma, Carlo Pierleoni, Aleksey N. Kolmogorov, Nikita Rybin, Dmitry Novoselov, Vladimir Anisimov, Artem R. Oganov, Chris J. Pickard, Tiange Bi, Ryotaro Arita, Ion Errea, Camilla Pellegrini, Ryan Requist, E. K. U. Gross, Elena Roxana Margine, Stephen R. Xie, Yundi Quan, Ajinkya Hire, Laura Fanfarillo, G. R. Stewart, J. J. Hamlin, Valentin Stanev, Renato S. Gonnelli, Erik Piatti, Davide Romanin, Dario Daghero, Roser Valenti
Summary: Designing materials with advanced functionalities, particularly ambient temperature superconductors, is a major focus of contemporary solid-state physics and chemistry. This article collects contributions from experts in the field to provide an overview of the current research status and roadmap for future theoretical and experimental challenges. Achieving ambient temperature superconductivity would not only open up exciting possibilities for fundamental research, but also have significant technological implications in areas such as energy conservation and climate change.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2022)
Article
Chemistry, Multidisciplinary
Corentin Jacquemmoz, Rituraj Mishra, Ludmilla Guduff, Carine van Heijenoort, Jean-Nicolas Dumez
Summary: Diffusion-ordered NMR spectroscopy (DOSY NMR) is a widely used method for the analysis of mixtures, allowing for the separation of spectra and analysis of interactions. Spatially-encoded (SPEN) DOSY enables the collection of a complete data set in less than 1 second, but there is a lack of thorough characterization of its features and practical use. Understanding the unusual principles and implementation of SPEN DOSY experiments is crucial for optimal utilization of the method in systems that evolve in time.
MAGNETIC RESONANCE IN CHEMISTRY
(2022)
Article
Chemistry, Physical
Jacob G. Lee, Chris J. Pickard, Bingqing Cheng
Summary: This study successfully simulated the high-pressure phase transition process of titanium dioxide at high temperatures by designing a machine learning potential based on an empirical model, and constructed a pressure-temperature phase diagram. The research results have important guiding significance for the synthesis and stabilization of high-pressure titanium dioxide phases.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Biochemical Research Methods
Rituraj Mishra, Jean-Nicolas Dumez
Summary: The article introduces a new method for using quadratic gradient spacing in diffusion NMR experiments, and its impact on the collection and analysis of diffusion data sets.
JOURNAL OF MAGNETIC RESONANCE
(2022)
Article
Physics, Multidisciplinary
Zihan Zhang, Tian Cui, Michael J. Hutcheon, Alice M. Shipley, Hao Song, Mingyang Du, Vladimir Z. Kresin, Defang Duan, Chris J. Pickard, Yansun Yao
Summary: Hydrogen-based superconductors offer a way to achieve room-temperature superconductivity, but their immediate application is limited by the high pressures required. This study proposes a strategy for designing high-temperature superconductors at low pressures by alloying small-radius elements and hydrogen to form ternary H-based superconductors with alloy backbones.
PHYSICAL REVIEW LETTERS
(2022)
Review
Chemistry, Physical
Celia Lhoste, Benjamin Lorandel, Clement Praud, Achille Marchand, Rituraj Mishra, Arnab Dey, Aurelie Bernard, Jean-Nicolas Dumez, Patrick Giraudeau
Summary: 2D NMR is widely used in various fields and has shown great potential for the study of complex biochemical or chemical mixtures. Ultrafast 2D NMR is a versatile approach that allows for the resolution of overlapped peaks in 1D spectra and provides both structural and quantitative information. It has undergone significant methodological developments and has become an efficient analytical tool with numerous applications in mixture analysis.
PROGRESS IN NUCLEAR MAGNETIC RESONANCE SPECTROSCOPY
(2022)
Article
Chemistry, Multidisciplinary
Achille Marchand, Rituraj Mishra, Aurelie Bernard, Jean-Nicolas Dumez
Summary: Online monitoring by flow NMR spectroscopy is a powerful tool for studying chemical reactions and processes, providing mechanistic understanding and driving optimizations. However, some useful methods for mixture analysis and reaction monitoring are not directly applicable in flow conditions. In this study, a fast and flow-compatible diffusion NMR experiment is described, allowing accurate diffusion data to be collected for samples flowing at up to 3 mL/min. This one-shot flow-compatible diffusion NMR opens up new possibilities for reaction monitoring applications.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Physics, Multidisciplinary
Cong Liu, Junjie Wang, Xin Deng, Xiaomeng Wang, Chris J. Pickard, Ravit Helled, Zhongqing Wu, Hui-Tian Wang, Dingyu Xing, Jian Sun
Summary: The reactivity and state of helium and silica under high pressure are crucial for understanding the evolution and internal structure of giant planets. By using calculations and predictions, researchers have identified four stable phases of a helium-silica compound with seven/eight-coordinated silicon atoms under the interior conditions of outer planets in the solar system. This compound exhibits different states in different planets, providing evidence for building more sophisticated interior models of giant planets.
CHINESE PHYSICS LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Margherita Bazzoni, Celia Lhoste, Justine Bonnet, Kouakou Eric Konan, Aurelie Bernard, Patrick Giraudeau, Francois-Xavier Felpin, Jean-Nicolas Dumez
Summary: This work demonstrates the online monitoring of a flow photochemical reaction using advanced NMR methods. By analyzing the reaction mixture directly, both 1D and ultrafast 2D experiments provide valuable information, especially for complex molecules. The study highlights the efficiency of ultrafast 2D COSY experiments for real-time monitoring and quantitative analysis, enabling effective screening of reaction conditions.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Rituraj Mishra, Jean-Nicolas Dumez
Summary: The measurement of translational diffusion coefficients by NMR spectroscopy is important in various fields and can be efficiently done using SPEN DNMR. However, motion other than diffusion can affect the accuracy of DNMR experiments, especially in the case of flow. This study provides a detailed theoretical analysis and numerical simulations to compensate for flow effects in SPEN DNMR experiments and evaluate their accuracy under different flow conditions.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Review
Biochemistry & Molecular Biology
Victor Ribay, Clement Praud, Marine P. M. Letertre, Jean-Nicolas Dumez, Patrick Giraudeau
Summary: Hyperpolarized NMR is a promising method to overcome the limited sensitivity of conventional NMR metabolomics in detecting minute metabolite concentrations in biological samples. This review discusses the utilization of dissolution dynamic nuclear polarization and parahydrogen-based techniques for molecular omics sciences, as well as recent advancements in combining hyperpolarization with fast multi-dimensional NMR and quantitative workflows. The review also proposes a comprehensive comparison of existing hyperpolarization techniques and addresses challenges in high throughput, sensitivity, and resolution for the general application of hyperpolarized NMR in metabolomics.
CURRENT OPINION IN CHEMICAL BIOLOGY
(2023)
Review
Chemistry, Multidisciplinary
Jean-Nicolas Dumez
Summary: NMR spectroscopy is a powerful method for analyzing mixtures, offering a wide range of methods and corresponding pulse sequences. This article describes various methods that address the complexity, low concentrations, and changing nature of mixtures. Examples from reaction monitoring and metabolomics are provided to illustrate the relevance and limitations of different methods.
CHEMICAL COMMUNICATIONS
(2022)
Article
Materials Science, Multidisciplinary
Chris J. Pickard
Summary: Structure prediction, which relies on the computation of energy landscapes, has become a crucial task in modern atomistic sciences. First-principles density functional calculations are highly reliable but computationally intensive. Machine learning potentials, or data derived potentials, offer a promising approach to describe entire energy landscapes at first-principles quality. Ab initio random structure searching is a powerful method for structure prediction, and a scheme compatible with it is described for the rapid construction of data derived potentials.
Article
Materials Science, Multidisciplinary
Jack Whaley-Baldwin, Chris J. Pickard
Summary: Using ab initio random structure searching (AIRSS), we performed a computational structure search and studied the phase diagram of elemental sulfur up to 100 TPa. Six new phases were discovered, with a transition sequence of bcc-I41/acd-cI16-α-U-hcp-A15-bcc. The critical temperature of sulfur superconductivity abruptly drops from 12 K to 0.4 K upon transition to the I41/acd phase at 1.24 TPa, and above 5 TPa, the critical temperature is found to be zero up to at least 100 TPa. The suppression of superconductivity is related to the formation of a sequence of electride phases with reduced electron-phonon coupling and charge localization.
Article
Chemistry, Physical
Hui Xie, Tianxiao Liang, Tian Cui, Xiaolei Feng, Hao Song, Da Li, Fubo Tian, Simon A. T. Redfern, Chris J. Pickard, Defang Duan
Summary: K2SiH6 is a promising hydrogen storage material with high hydrogen density and appropriate dehydrogenation temperature. Other potential hydrogen storage materials have also been found, which require further investigation under high pressure.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
