The field of computational chemistry has made an impressive impact on contemporary chemical research. In order to carry out computational studies on actual systems, sophisticated software is required in form of large-scale quantum chemical program packages. Given the enormous diversity and complexity of the methods that need to be implementation in such packages, it is evident that these software pieces are very large (millions of code lines) and extremely complex. Most of the packages in widespread use by the computational chemistry community have had a development history of decades. Given the rapid progress in the hardware and a lack of resources (time, workforce, money), it is not possible to keep redesigning these program packages from scratch in order to keep up with the ever more quickly shifting hardware landscape. In this perspective, some aspects of the multitude of challenges that the developer community faces are discussed. While the task at hand - to ensure that quantum chemical program packages can keep evolving and make best use of the available hardware - is daunting, there are also new evolving opportunities. The problems and potential cures are discussed with the example of the ORCA package that has been developed in our research group.
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http://dx.doi.org/10.1039/d4fd00056k | DOI Listing |
Adv Mater
March 2025
Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore, 117585, Republic of Singapore.
Tuning transition metal spin states potentially offers a powerful means to control electrocatalyst activity. However, implementing such a strategy in electrochemical CO reduction (COR) is challenging since rational design rules have yet to be elucidated. Here we show how the addition of P dopants to a ferromagnetic element (Fe, Co, and Ni) single-atom catalyst (SAC) can shift its spin state.
View Article and Find Full Text PDFChempluschem
March 2025
Malaviya National Institute of Technology Jaipur, Chemistry, INDIA.
The present work investigates the impact of the external electric field (EEF) on the oxidizing power of N 2 O, by employing kinetics and quantum chemical calculations. We have taken the oxidation of olefin (Ethene and cyclohexene) by N 2 O as a prototype to demonstrate the effectiveness of EEF. The investigation suggests that the reaction barrier is significantly reduced by choosing an electric field in an appropriate direction.
View Article and Find Full Text PDFMaterials (Basel)
February 2025
Centre for Quantum Physics, Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurement (MOE), School of Physics, Beijing Institute of Technology, Beijing 100081, China.
A topological insulator with large bulk-insulating behavior and high electron mobility of the surface state is needed urgently, not only because it would be a good platform for studying topological surface states but also because it is a prerequisite for potential future applications. In this work, we demonstrated that tin (Sn) or indium (In) dopants could be introduced into a BiSbTeSe single crystal. The impacts of the dopants on the bulk-insulating property and electron mobility of the surface state were systematically investigated by electrical transport measurements.
View Article and Find Full Text PDFMaterials (Basel)
February 2025
School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
To explore the impact of different substituents (R) in 4-R-1,5-diaminotetrazolium cations on the performance of their pentazolate salts, five types of pentazolate salts with different groups were designed: -H, -OH, -NH, -NH-NH, and -N. Quantum chemical methods were employed to deeply study the interionic interactions and detonation properties of these 4-R-1,5-diaminotetrazolium pentazolate salts. Among these five ionic compounds, the 1,5-diamino-4-hydroxytetrazolium pentazolate ([DAT-OH] [N]) system exhibited the lowest interaction energy and highest stability, while the 1,5-diamino-1H-1,2,3,4-tetrazolium pentazolate ([DAT-H] [N]) system was the least stable.
View Article and Find Full Text PDFMolecules
March 2025
Department of Physics, Graduate School of Science, Tohoku University, Sendai 980-8578, Japan.
This article provides a comprehensive review of quantum chemical computational studies on the thermal and photochemical reactions of organosilicon compounds, based on fundamental concepts such as initial complex formation, HOMO-LUMO interactions, and subjacent orbital interactions. Despite silicon's position in group 14 of the periodic table, alongside carbon, its reactivity patterns exhibit significant deviations from those of carbon. This review delves into the reactivity behaviors of organosilicon compounds, particularly focusing on the highly coordinated nature of silicon.
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