The Best of Both Worlds: ΔDFT Describes Multiresonance TADF Emitters with Wave-Function Accuracy at Density-Functional Cost

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер unknown, С. 1114 - 1125

Опубликована: Янв. 23, 2025

With their narrow-band emission, high quantum yield, and good chemical stability, multiresonance thermally activated delayed fluorescence (MR-TADF) emitters are promising materials for OLED technology. However, accurately modeling key properties, such as the singlet-triplet (ST) energy gap energy, remains challenging. While time-dependent density functional theory (TD-DFT), workhorse of computational science, suffers from fundamental issues, wave function-based coupled-cluster (CC) approaches, like approximate CC second-order (CC2), accurate but suffer cost unfavorable scaling with system size. This work demonstrates that a state-specific ΔDFT approach based on unrestricted Kohn-Sham (ΔUKS) combines best both worlds: diverse benchmark set 35 MR-TADF emitters, ΔUKS performs or better than CC2, recovering experimental ST gaps mean absolute deviation (MAD) 0.03 eV at small fraction CC2. When combined tuned range-separated LC-ωPBE functional, excellent performance extends to energies MR- donor-acceptor TADF even molecules an inverted (INVEST), rendering this jack all trades organic electronics.

Язык: Английский

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Crash testing machine learning force fields for molecules, materials, and interfaces: model analysis in the TEA Challenge 2023

Chemical Science, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Assessing the performance of modern machine learning force fields across diverse chemical systems to identify their strengths and limitations within TEA Challenge 2023.

Язык: Английский

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Quantum mechanical-based strategies in drug discovery: Finding the pace to new challenges in drug design

Current Opinion in Structural Biology, Год журнала: 2024, Номер 87, С. 102870 - 102870

Опубликована: Июнь 24, 2024

The expansion of the chemical space to tangible libraries containing billions synthesizable molecules opens exciting opportunities for drug discovery, but also challenges power computer-aided design prioritize best candidates. This directly hits quantum mechanics (QM) methods, which provide chemically accurate properties, subject small-sized systems. Preserving accuracy while optimizing computational cost is at heart many efforts develop high-quality, efficient QM-based strategies, reflected in refined algorithms and approaches. QM-tailored physics-based force fields coupling QM with machine learning, conjunction computing performance supercomputing resources, will enhance ability use these methods discovery. challenge formidable, we undoubtedly see impressive advances that define a new era.

Язык: Английский

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Extension of the D3 and D4 London Dispersion Corrections to the full Actinides Series

Physical Chemistry Chemical Physics, Год журнала: 2024, Номер 26(32), С. 21379 - 21394

Опубликована: Янв. 1, 2024

Efficient dispersion corrections are an indispensable component of modern density functional theory, semi-empirical quantum mechanical, and even force field methods. In this work, we extend the well established D3 D4 London to full actinides series, francium, radium. To keep consistency with existing versions, original parameterization strategy model was only slightly modified. This includes improved reference Hirshfeld atomic partial charges at ωB97M-V/ma-def-TZVP level fit required electronegativity equilibration charge (EEQ) model. context, developed a new actinide data set called AcQM, which covers most common molecular compound space. Furthermore, efficient calculation dynamic polarizabilities that needed construct

Язык: Английский

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Analyzing the Linker Structure of PROTACs throughout the Induction Process: Computational Insights

Journal of Medicinal Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Янв. 29, 2025

Linker structures are a crucial component of proteolysis-targeting chimeras (PROTACs) and have traditionally been designed based on empirical methods, which presents significant challenges in the development PROTACs. Current optimization strategies typically focus reducing number rotatable bonds linker to limit conformational freedom. However, this approach overlooks complexity target protein degradation process. Retrospective analyses suggest that merely adjusting is insufficient control freedom PROTACs, indicating need for new strategies. By integration computational methods such as molecular dynamics simulations, study investigates role throughout induction process, particularly its impact formation stability ternary complex. This offers potential overcoming limitations traditional strategies, reliance enhancing overall efficiency effectiveness PROTAC design.

Язык: Английский

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Overview on Building Blocks and Applications of Efficient and Robust Extended Tight Binding

The Journal of Physical Chemistry A, Год журнала: 2025, Номер unknown

Опубликована: Фев. 27, 2025

The extended tight binding (xTB) family of methods opened many new possibilities in the field computational chemistry. Within just 5 years, GFN2-xTB parametrization for all elements up to Z = 86 enabled more than a thousand applications, which were previously not feasible with other electronic structure methods. xTB provide robust and efficient way apply quantum mechanics-based approaches obtaining molecular geometries, computing free energy corrections or describing noncovalent interactions found applicability targets. A crucial contribution success is availability within simulation packages frameworks, supported by open source development its program library packages. We present comprehensive summary applications capabilities different fields Moreover, we consider main software calculations, covering their current ecosystem, novel features, usage scientific community.

Язык: Английский

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Potent SARS-CoV-2 3C-like protease inhibitor ( +)-eupenoxide-3,6-diketone (IC50: 0.048 μM) was synthesized based on ( +)-eupenoxide; lead from ( +)-eupenoxide analogs study by endophytic fermentation

Journal of Natural Medicines, Год журнала: 2025, Номер 79(2), С. 357 - 370

Опубликована: Фев. 3, 2025

Язык: Английский

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Decoding Solubility Signatures from Amyloid Monomer Energy Landscapes

Journal of Chemical Theory and Computation, Год журнала: 2025, Номер unknown

Опубликована: Фев. 24, 2025

This study investigates the energy landscapes of amyloid monomers, which are crucial for understanding protein misfolding mechanisms in Alzheimer's disease. While proteins possess inherent thermodynamic stability, environmental factors can induce deviations from native folding pathways, leading to and aggregation, phenomena closely linked solubility. Using UNOPTIM program, integrates UNRES potential into Cambridge landscape framework, we conducted single-ended transition state searches employed discrete path sampling compute kinetic networks starting PDB structures. These consist local minima states that connect them, quantify monomers. We defined clusters within each using thresholds selected their lowest-energy structures structural analysis. Applying graph convolutional networks, identified solubility trends correlated them with features. Our findings identify specific low solubility, characteristic aggregation-prone states, highlighting key residues drive reduced Notably, exposure hydrophobic residue Phe19 solvent triggers a collapse by disrupting neighboring helix. Additionally, investigated determine first passage times between thereby elucidating kinetics these landscapes. comprehensive approach provides valuable insights thermodynamics Aβ By integration multiple analytical techniques explore landscapes, our features associated have inform future therapeutic strategies aimed at addressing aggregation neurodegenerative diseases.

Язык: Английский

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From Ab Initio to Instrumentation: A Field Guide to Characterizing Multivalent Liquid Electrolytes

Chemical Reviews, Год журнала: 2025, Номер unknown

Опубликована: Март 10, 2025

In this field guide, we outline empirical and theory-based approaches to characterize the fundamental properties of liquid multivalent-ion battery electrolytes, including (i) structure chemistry, (ii) transport, (iii) electrochemical properties. When detailed molecular-scale understanding multivalent electrolyte behavior is insufficient use examples from well-studied lithium-ion electrolytes. recognition that coupling techniques highly effective, but often nontrivial, also highlight recent characterization efforts uncover a more comprehensive nuanced underlying structures, processes, reactions drive performance system-level behavior. We hope insights these discussions will guide design future studies, accelerate development next-generation batteries through modeling with experiments, help avoid pitfalls ensure reproducibility results.

Язык: Английский

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Quantum chemical package Jaguar: A survey of recent developments and unique features

The Journal of Chemical Physics, Год журнала: 2024, Номер 161(5)

Опубликована: Авг. 2, 2024

This paper is dedicated to the quantum chemical package Jaguar, which commercial software developed and distributed by Schrödinger, Inc. We discuss Jaguar’s scientific features that are relevant research as well describe those aspects of program pertinent user interface, organization computer code, its maintenance testing. Among topics feature prominently in this methods grounded pseudospectral approach. A number multistep workflows dependent on Jaguar covered: prediction protonation equilibria aqueous solutions (particularly calculations tautomeric stability pKa), reactivity predictions based automated transition state search, assembly Boltzmann-averaged spectra such vibrational electronic circular dichroism, nuclear magnetic resonance. Discussed also oriented toward materials science applications, particular, properties optoelectronic organic semiconductors, molecular catalyst design. The topic treatment conformations inevitably comes up real world projects considered part all mentioned above. In addition, we examine role machine learning performed from auxiliary functions return approximate calculation runtime a actual properties. current work second series reviews first having been published more than ten years ago. Thus, serves rare milestone path being traversed development thirty existence.

Язык: Английский

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