Best‐Practice DFT Protocols for Basic Molecular Computational Chemistry**

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(42)

Опубликована: Сен. 14, 2022

Nowadays, many chemical investigations are supported by routine calculations of molecular structures, reaction energies, barrier heights, and spectroscopic properties. The lion's share these quantum-chemical applies density functional theory (DFT) evaluated in atomic-orbital basis sets. This work provides best-practice guidance on the numerous methodological technical aspects DFT three parts: Firstly, we set stage introduce a step-by-step decision tree to choose computational protocol that models experiment as closely possible. Secondly, present recommendation matrix guide choice depending task at hand. A particular focus is achieving an optimal balance between accuracy, robustness, efficiency through multi-level approaches. Finally, discuss selected representative examples illustrate recommended protocols effect choices.

Язык: Английский

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Best‐Practice DFT Protocols for Basic Molecular Computational Chemistry**

Angewandte Chemie, Год журнала: 2022, Номер 134(42)

Опубликована: Сен. 14, 2022

Abstract Nowadays, many chemical investigations are supported by routine calculations of molecular structures, reaction energies, barrier heights, and spectroscopic properties. The lion's share these quantum‐chemical applies density functional theory (DFT) evaluated in atomic‐orbital basis sets. This work provides best‐practice guidance on the numerous methodological technical aspects DFT three parts: Firstly, we set stage introduce a step‐by‐step decision tree to choose computational protocol that models experiment as closely possible. Secondly, present recommendation matrix guide choice depending task at hand. A particular focus is achieving an optimal balance between accuracy, robustness, efficiency through multi‐level approaches. Finally, discuss selected representative examples illustrate recommended protocols effect choices.

Язык: Английский

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Contemporary Quantum Computing Use Cases: Taxonomy, Review and Challenges

Archives of Computational Methods in Engineering, Год журнала: 2022, Номер 30(1), С. 615 - 638

Опубликована: Сен. 26, 2022

Язык: Английский

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Meta-GGA Density Functional Calculations on Atoms with Spherically Symmetric Densities in the Finite Element Formalism

Journal of Chemical Theory and Computation, Год журнала: 2023, Номер 19(9), С. 2502 - 2517

Опубликована: Апрель 21, 2023

Density functional calculations on atoms are often used for determining accurate initial guesses as well generating various types of pseudopotential approximations and efficient atomic-orbital basis sets polyatomic calculations. To reach the best accuracy these purposes, atomic should employ same density calculation. Atomic typically carried out employing spherically symmetric densities, corresponding to use fractional orbital occupations. We have described their implementation (DFAs) belonging local approximation (LDA) generalized gradient (GGA) levels theory Hartree–Fock (HF) range-separated exact exchange [Lehtola, S. Phys. Rev. A 2020, 101, 012516]. In this work, we describe extension meta-GGA functionals using Kohn–Sham scheme, in which energy is minimized with respect orbitals, turn expanded finite element formalism high-order numerical functions. Furnished new implementation, continue our recent work well-behavedness S.; Marques, M. A. L. J. Chem. 2022, 157, 174114]. pursue complete set (CBS) limit energies find many be ill-behaved Li Na atoms. report truncation errors (BSTEs) some commonly Gaussian BSTEs strongly dependent. also discuss importance thresholding DFAs that all studied yield total converged 0.1 μEh when densities smaller than 10–11a0–3 screened out.

Язык: Английский

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Atomic Electronic Structure Calculations with Hermite Interpolating Polynomials

The Journal of Physical Chemistry A, Год журнала: 2023, Номер 127(18), С. 4180 - 4193

Опубликована: Апрель 27, 2023

We have recently described the implementation of atomic electronic structure calculations within finite element method with numerical radial basis functions form χμ(r) = r–1Bμ(r), where high-order Lagrange interpolating polynomials (LIPs) were used as shape Bμ(r). In this work, we discuss how can be evaluated in a stable manner at small r and also revisit choice Three kinds are considered: addition to C0 continuous LIPs, consider analytical first-order Hermite (HIPs) that C1 continuous, well implementations n-th order (Cn continuous) HIPs expressed terms an underlying LIP basis. Furnished new implementation, demonstrate reliable even large numbers nodes they work nonuniform grids, affording better results than LIPs same total number functions. discontinuities observed spin-σ local kinetic energy τσ sets, while HIP sets do not suffer from such issues; however, either set reach complete limit smooth τσ. Moreover, implications on meta-GGA functionals recent functionals, find most Minnesota ill-behaved. examine potential usefulness explicit control over derivative for forming orbital but confining potentials still likely option.

Язык: Английский

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Smartphones as a platform for molecular analysis: concepts, methods, devices and future potential

Lab on a Chip, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Smartphones have the potential to transform chemical and biological analysis by functioning as portable, versatile, democratized platforms for molecular diagnostics. Recent advances in optical detection devices are reviewed.

Язык: Английский

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Vision 2050: Reaction Engineering Roadmap

ACS Engineering Au, Год журнала: 2023, Номер 3(6), С. 364 - 390

Опубликована: Окт. 22, 2023

This perspective provides the collective opinions of a dozen chemical reaction engineers from academia and industry. In this sequel to "Vision 2020: Reaction Engineering Roadmap," published in 2001, we provide our about field engineering by addressing current situation, identifying barriers progress, recommending research directions context four industry sectors (basic chemicals, specialty pharmaceuticals, polymers) five technology areas (reactor system selection, design scale-up, mechanism development property estimation, catalysis, nonstandard reactor types, electrochemical systems). Our input report includes numerous recommendations regarding needs coming decades, including guidance for prioritizing efforts workforce development, measurement science, computational methods. We see important roles plastics circularity challenge, decarbonization processes, electrification reactors, conversion batch processes continuous intensified, dynamic processes.

Язык: Английский

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Structural, mechanical, electronic and optical properties of MFe2O4(M=Zn, Cu, Si) ferrites for electrochemical, photocatalytic and optoelectronic applications

Journal of Solid State Chemistry, Год журнала: 2023, Номер 330, С. 124504 - 124504

Опубликована: Дек. 13, 2023

Язык: Английский

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A call to arms: Making the case for more reusable libraries

The Journal of Chemical Physics, Год журнала: 2023, Номер 159(18)

Опубликована: Ноя. 10, 2023

The traditional foundation of science lies on the cornerstones theory and experiment. Theory is used to explain experiment, which in turn guides development theory. Since advent computers computational algorithms, computation has risen as third cornerstone science, joining experiment an equal footing. Computation become essential part modern amending by enabling accurate comparison complicated theories sophisticated experiments, well guiding triage both design targets experiments novel methods. Like relies continued investment infrastructure: it requires hardware (the physical computer calculation run) software source code programs that performs wanted simulations). In this Perspective, I discuss present-day challenges side chemistry, arise from fast-paced programming models, hardware. argue many these could be solved with reusable open libraries, are a public good, enhance reproducibility accelerate availability state-of-the-art methods improved software.

Язык: Английский

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eChem: A Notebook Exploration of Quantum Chemistry

Journal of Chemical Education, Год журнала: 2023, Номер 100(4), С. 1664 - 1671

Опубликована: Март 15, 2023

The eChem project features an e-book published as a web page (10.30746/978-91-988114-0-7), collecting repository of Jupyter notebooks developed for the dual purpose explaining and exploring theory underlying computational chemistry in highly interactive manner well providing tutorial-based presentation complex workflows needed to simulate embedded molecular systems real biochemical and/or technical interest. For students ranging from beginners advanced users, book is suited self-directed learning, but workshops led by experienced instructors targeting student bodies with specific needs interests can readily be formed its components. This has been done using base workshop directed toward graduate learning practices quantum chemistry, resulting very positive assessment nature this framework. members team are engaged both education research, mirroring activity, we develop open-source software upon which predominantly based. overarching vision goal our work provide science- education-enabling platform modeling on contemporary future high-performance computing systems, document development book.

Язык: Английский

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