Polymer Matrix Drives Dual Phosphorescence in Dispersed Chromophores DOI Creative Commons

Pakkirisamy Thilagar,

Subhajit Ghosh Ghosh,

Rajendra Prasad Nandi

и другие.

Research Square (Research Square), Год журнала: 2025, Номер unknown

Опубликована: Фев. 13, 2025

Abstract Poly(methyl methacrylate) (PMMA) matrix has been extensively explored for decades to achieve efficient room-temperature phosphorescence in blue-to-red regions from dispersed chromophores. Isolated chromophores at low-weight concentrations the polymer eliminate inter-chromophore interactions. However, impact of on optical characteristics remains elusive. Herein, we analyze dual behavior three molecularly (1 wt.% concentration) PMMA matrix. We employ second-order Algebraic Diagrammatic Construction (ADC2) excited state calculations show that observed BANHPh and BANMePh does not stem T1 T2 electronic states. Instead, this phenomenon arises matrix-assisted, accessible conformers within (T1H T1L). The creates an asymmetric environment around chromophores, inducing structural modulations result spectral tuning singlet triplet manifolds. In conclusion, conformation-dependent is unlikely occur without These matrix-induced phosphorescent emitters have demonstrated be highly competent application fingerprint recognition, information encryption, afterglow display.

Язык: Английский

Crash testing machine learning force fields for molecules, materials, and interfaces: model analysis in the TEA Challenge 2023 DOI Creative Commons
Igor Poltavsky, Anton Charkin-Gorbulin, Mirela Puleva

и другие.

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

Процитировано

2
Extension of the D3 and D4 London Dispersion Corrections to the full Actinides Series DOI Creative Commons
Lukas Wittmann, Igor Gordiy, Marvin Friede

и другие.

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

Процитировано

12
Quantum mechanical-based strategies in drug discovery: Finding the pace to new challenges in drug design DOI Creative Commons
Tiziana Ginex, Javier Vázquez,

Carolina Estarellas

и другие.

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

Процитировано

11
Accurate Enthalpies of Formation for Bioactive Compounds from High-Level Ab Initio Calculations with Detailed Conformational Treatment: A Case of Cannabinoids DOI

Andrei F. Kazakov,

Eugene Paulechka

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

Опубликована: Янв. 9, 2025

Our recently developed approach based on the local coupled-cluster with single, double, and perturbative triple excitation [LCCSD(T)] model gives very efficient means to compute ideal-gas enthalpies of formation. The expanded uncertainty (95% confidence) method is about 3 kJ·mol–1 for medium-sized compounds, comparable typical experimental measurements. Larger compounds interest often exhibit many conformations that can significantly differ in intramolecular interactions. Although present capabilities allow processing even a few hundred distinct conformer structures given compound, systems numbers well excess 1000. In this study, we investigate how reduce number expensive LCCSD(T) calculations large ensembles while controlling error approximation. best strategy found was correct results lower-level, surrogate (density functional theory, DFT) systematic manner. It also conformational contribution introduced by mainly driven (bias) rather than random component DFT energy deviation from target. This distinction usually overlooked benchmarking studies. As result work, formation 20 cannabinoid cannabinoid-related were obtained. Comprehensive analysis suggests uncertainties obtained values are below 4 kJ·mol–1.

Язык: Английский

Процитировано

1
The Best of Both Worlds: ΔDFT Describes Multiresonance TADF Emitters with Wave-Function Accuracy at Density-Functional Cost DOI
Lukas Kunze, Andreas Hansen, Stefan Grimme

и другие.

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

Процитировано

1
Analyzing the Linker Structure of PROTACs throughout the Induction Process: Computational Insights DOI

Yihao Li,

Xiaoxuan Zhang, Jiali Xie

и другие.

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

Процитировано

1
Benchmarking Molecular and Periodic Extended Tight Binding Methods for Spin-State Energies in Spin-Crossover Systems DOI
Silvia Gómez‐Coca, Eliseo Ruíz

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

Опубликована: Фев. 13, 2025

Язык: Английский

Процитировано

1
From Ab Initio to Instrumentation: A Field Guide to Characterizing Multivalent Liquid Electrolytes DOI
Glenn Pastel, Travis P. Pollard,

Oleg Borodin

и другие.

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

Процитировано

1
Multilevel Framework for Analysis of Protein Folding Involving Disulfide Bond Formation DOI Creative Commons
Patryk A. Wesołowski, David J. Wales, Philipp Pracht

и другие.

The Journal of Physical Chemistry B, Год журнала: 2024, Номер 128(13), С. 3145 - 3156

Опубликована: Март 21, 2024

In this study, a three-layered multicenter ONIOM approach is implemented to characterize the naive folding pathway of bovine pancreatic trypsin inhibitor (BPTI). Each layer represents distinct level theory, where initial layer, encompassing entire protein, modeled by general all-atom force-field GFN-FF. An intermediate electronic structure consisting three fragments introduced with state-of-the-art semiempirical tight-binding method GFN2-xTB. Higher accuracy, specifically addressing breaking and formation disulfide bonds, achieved at innermost using composite DFT r2SCAN-3c. Our analysis sheds light on structural stability BPTI, particularly significance interlinking bonds. The accuracy efficiency QM/SQM/MM are benchmarked oxidative cystine. For relative stabilities investigated through calculation free energy contributions for selected intermediates, focusing impact bond. results highlight intricate trade-off between computational cost, demonstrating that provides well-balanced comprehensive solution describe effects in biomolecular systems. We conclude multiscale landscape exploration robust methodology study intriguing biological targets.

Язык: Английский

Процитировано

6
Reparameterization of GFN1-xTB for atmospheric molecular clusters: applications to multi-acid–multi-base systems DOI Creative Commons
Yosef Knattrup, Jakub Kubečka, Haide Wu

и другие.

RSC Advances, Год журнала: 2024, Номер 14(28), С. 20048 - 20055

Опубликована: Янв. 1, 2024

Reparameterization of GFN1-xTB for atmospheric molecular clusters leads to a massive decrease in energy errors and deviation.

Язык: Английский

Процитировано

5