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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A Guide to In Silico Drug Design

Pharmaceutics, Год журнала: 2022, Номер 15(1), С. 49 - 49

Опубликована: Дек. 23, 2022

The drug discovery process is a rocky path that full of challenges, with the result very few candidates progress from hit compound to commercially available product, often due factors, such as poor binding affinity, off-target effects, or physicochemical properties, solubility stability. This further complicated by high research and development costs time requirements. It thus important optimise every step in order maximise chances success. As recent advancements computer power technology, computer-aided design (CADD) has become an integral part modern guide accelerate process. In this review, we present overview CADD methods applications, silico structure prediction, refinement, modelling target validation, are commonly used area.

Язык: Английский

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Review on multi-dimensional assembled S-scheme heterojunction photocatalysts

Journal of Material Science and Technology, Год журнала: 2023, Номер 160, С. 214 - 239

Опубликована: Апрель 23, 2023

Язык: Английский

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CREST—A program for the exploration of low-energy molecular chemical space

The Journal of Chemical Physics, Год журнала: 2024, Номер 160(11)

Опубликована: Март 21, 2024

Conformer–rotamer sampling tool (CREST) is an open-source program for the efficient and automated exploration of molecular chemical space. Originally developed in Pracht et al. [Phys. Chem. Phys. 22, 7169 (2020)] as driver calculations at extended tight-binding level (xTB), it offers a variety molecular- metadynamics simulations, geometry optimization, structure analysis capabilities. Implemented algorithms include procedures conformational sampling, explicit solvation studies, calculation absolute entropy, identification protonation deprotonation sites. Calculations are set up to run concurrently, providing single-node parallelization. CREST designed require minimal user input comes with implementation GFNn-xTB Hamiltonians GFN-FF force-field. Furthermore, interfaces any quantum chemistry force-field software can easily be created. In this article, we present recent developments code show selection applications most important features program. An novelty refactored backend, which provides significant speed-up small or medium-sized drug molecules allows more sophisticated setups, example, mechanics/molecular mechanics minimum energy crossing point calculations.

Язык: Английский

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A direct observation of up-converted room-temperature phosphorescence in an anti-Kasha dopant-matrix system

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Апрель 8, 2023

It is common sense that emission maxima of phosphorescence spectra (λP) are longer than those fluorescence (λF). Here we report a serendipitous finding up-converted room-temperature (RTP) with λP < λF and lifetime > 0.1 s upon doping benzophenone-containing difluoroboron β-diketonate (BPBF2) into phenyl benzoate matrices. The RTP originated from BPBF2's Tn (n ≥ 2) states which show typical 3n-π* characters benzophenone moieties. Detailed studies reveal that, intersystem crossing S1 charge transfer characters, the resultant T1 build T1-to-Tn equilibrium. Because their possess large rates can strongly compete RTP(T1) to directly emit RTP(Tn) violates Kasha's rule. direct observation provides deep understanding triplet excited state dynamics opens an intriguing pathway devise visible-light-excitable deep-blue afterglow emitters, as well stimuli-responsive materials.

Язык: Английский

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Electrochemical surface-enhanced Raman spectroscopy

Nature Reviews Methods Primers, Год журнала: 2023, Номер 3(1)

Опубликована: Окт. 26, 2023

Язык: Английский

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Density functional theory methods applied to homogeneous and heterogeneous catalysis: a short review and a practical user guide

Physical Chemistry Chemical Physics, Год журнала: 2024, Номер 26(10), С. 7950 - 7970

Опубликована: Янв. 1, 2024

The application of density functional theory (DFT) methods in catalysis has been growing fast the last few decades thanks to both availability more powerful high computing resources and development new efficient approximations approaches. DFT calculations allow for understanding crucial catalytic aspects that are difficult or even impossible access by experiments, thus contributing faster selective catalysts. Depending on system properties under investigation, different approaches should be used. Moreover, reliability obtained results deeply depends involved selected method model. This review addresses chemists, physicists materials scientists whose interest deals with DFT-based computational tools homogeneous heterogeneous catalysis. First, a brief introduction is presented. Then, main based atomic centered basis sets plane waves discussed, underlining differences, advantages limitations. Eventually, guidance towards selection model given, final focus evaluation energy barriers, which represents step all processes. Overall, rational practical guide beginners experienced users wide field

Язык: Английский

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DFT-Enabled Development of Hemilabile (P^∧N) Ligands for Gold(I/III) RedOx Catalysis: Application to the Thiotosylation of Aryl Iodides

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(6), С. 3660 - 3674

Опубликована: Фев. 5, 2024

Ligand-enabled oxidative addition of Csp2-X bonds to Au(I) centers has recently appeared as a valuable strategy for the development catalytic RedOx processes. Several cross-coupling reactions that were previously considered difficult achieve reported lately, thus expanding synthetic potential gold(I) complexes beyond traditional nucleophilic functionalization π-systems. MeDalPhos played an important role in this and, despite several studies on alternative structures, remains, so far, only general ligand such process. We report herein discovery and DFT-enabled structural optimization new family hemilabile (P∧N) ligands can promote aryl iodides gold(I). These flexible ligands, which possess common 2-methylamino heteroaromatic N-donor motif, are structurally electronically tunable, being easily accessible affordable. The corresponding shown outperform reactivity (MeDalPhos)Au(I) series alkoxy- amidoarylations alkenes. Their comparatively higher further highlighted thiotosylation iodides, challenging unreported C–S reaction could not be achieved under classical Pd(0/II) catalysis allows divergent access sulfur derivatives.

Язык: Английский

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Transition Metal Molybdates Emerging Materials for High‐Performance Supercapacitors: A Machine Learning Analysis

Battery energy, Год журнала: 2025, Номер unknown

Опубликована: Янв. 19, 2025

ABSTRACT Transition metal molybdates (AMoO 4 where A = Ni, Co, Mn, Fe, and Zn) have attracted much attention as promising electrode materials for energy storage devices due to their multi‐electron redox capability, higher electrical conductivity, good chemical thermal stability, stable crystal structure get superior electrochemical performance. graphene‐based composites possess multidimensional morphology supercapacitors. The morphology‐dependent supercapacitor behavior has been reviewed in the present article. formation mechanism of AMoO nanostructures form 1D, 2D, 3D identified respective is outlined. density functional theory based on calculated electronic properties discussed. Additionally, application machine learning techniques predicting analyzing relationships discussed first time. By leveraging ML algorithms, we identify key parameters influencing capabilities, providing insights into rational design molybdate‐based composites. Integrating experimental results with ML‐driven optimization offers a novel pathway accelerating development next‐generation devices. In conclusion, future perspectives challenges

Язык: Английский

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ωB97X-3c: A composite range-separated hybrid DFT method with a molecule-optimized polarized valence double-ζ basis set

The Journal of Chemical Physics, Год журнала: 2022, Номер 158(1)

Опубликована: Дек. 12, 2022

A new composite density functional theory (DFT) method is presented. It based on ωB97X-V as one of the best-performing functionals for GMTKN55 thermochemistry database and completes family "3c" methods toward range-separated hybrid DFT. This consistently available all elements up to Rn (Z = 1-86). Its further key ingredients are a polarized valence double-ζ (vDZP) Gaussian basis set, which was fully optimized in molecular DFT calculations, combination with large-core effective core potentials specially adapted D4 dispersion correction. Unlike most existing atomic orbital sets, vDZP shows only small set superposition errors (BSSEs) can compete standard sets triple-ζ quality. Small residual BSSE effects efficiently absorbed by damping scheme, overall eliminates need an explicit treatment or empirical corrections BSSE. Thorough tests variety benchmark show that method, dubbed ωB97X-3c, par even outperforms quadruple-zeta at fraction computational cost. Particular strengths this description non-covalent interactions barrier heights, it among overall.

Язык: Английский

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