Computing Excited States of Very Large Systems with Range-Separated Hybrid Functionals and the Exact Integral Simplified Time-Dependent Density Functional Theory (XsTD-DFT) DOI
Marc de Wergifosse

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: unknown, P. 12628 - 12635

Published: Dec. 17, 2024

Simplified quantum chemistry (sQC) methods can routinely compute excited states for very large systems in an "all-atom" fashion. They are viable alternatives to regular multiscale schemes. sQC have the advantage of accounting explicitly all environment at a mechanical (QM) level. The treatment charge-transfer is now improved by native implementation range-separated hybrid (RSH) exchange-correlation functionals into eXact integral simplified time-dependent density functional theory (XsTD-DFT). After RSH XsTD-DFT/TDA scheme was benchmarked, XsTD-DFT(/TDA) ultraviolet/visible absorption, circular dichroism (CD), and/or two-photon absorption (2PA) spectra were directly compared results experiments four challenging and increasingly systems: eYFP model system, Λ-shaped multimodular D-π-A-π-D'-π-A-π-D chromophore, mixed donor/acceptor ligand Pd(II) double cage [3BF

Language: Английский

Cocrystals of axially N-embedded quasi-carbon nanohoops via modulating the electron affinity of guest acceptors DOI
Li Zhang, Shuhai Qiu,

Shunlong Hu

et al.

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 16, 2025

Language: Английский

Citations

1

Recent Progress of Chemical Reactions Induced by Contact Electrification DOI Creative Commons
Xiaolin Huo, Shaoxin Li, Bing Sun

et al.

Molecules, Journal Year: 2025, Volume and Issue: 30(3), P. 584 - 584

Published: Jan. 27, 2025

Contact electrification (CE) spans from atomic to macroscopic scales, facilitating charge transfer between materials upon contact. This interfacial exchange, occurring in solid–solid (S–S) or solid–liquid (S–L) systems, initiates radical generation and chemical reactions, collectively termed contact-electro-chemistry (CE-Chemistry). As an emerging platform for green chemistry, CE-Chemistry facilitates redox, luminescent, synthetic, catalytic reactions without the need external power sources as traditional electrochemistry with noble metal catalysts, significantly reducing energy consumption environmental impact. Despite its broad applicability, mechanistic understanding of remains incomplete. In S–S is primarily driven by surface charges, whether electrons, ions, radicals, on charged solid interfaces. However, a comprehensive theoretical framework yet be established. While CE offers promising exploring interplay triboelectric via modulation, it faces significant challenges achieving scalability optimizing efficiency. contrast, S–L focuses electron critical step subsequent reactions. approach notably versatile, enabling bulk-phase solutions offering flexibility choose various solvents and/or dielectrics optimize reaction pathways, such degradation organic pollutants polymerization, etc. The formation electrical double layer (EDL), ion adsorption following transfer, plays pivotal role CE-Chemical processes within aqueous systems. EDL can exert screening effect further thereby inhibiting progress. A optimization mechanisms are elucidating pathways precise control over processes. foundation CE-Chemistry, underpins development energy-efficient environmentally sustainable methodologies, holding transformative potential advancing innovation. review consolidates recent advancements, systematically classifying progress based configurations systems underlying dynamics. To unlock full future research should prioritize strategic tuning material electronegativity, engineering sophisticated architectures, enhancement transport mechanisms, paving way innovations.

Language: Английский

Citations

1

Buckybowl‐Based Fullerene Receptors DOI

Wenru Song,

Xiangfeng Shao

Chemistry - A European Journal, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 24, 2024

Abstract Buckybowls, bowl‐shaped polyaromatic hydrocarbons, have received intensive interest owing to their multifaceted potentials in supramolecular chemistry and materials science. Buckybowls possess unique chemical physical properties associated with concave convex faces. In view of the shape complementarity, which is one key factors for host‐guest assembly, buckybowls are ideal receptors fullerenes. fact, assembly between fullerenes most active topics chemistry, resulting show promising applications optoelectronics, biomaterials, so forth. this tutorial review, we present an overview progress on fullerene based over last decade.

Language: Английский

Citations

4

Computational investigation of the perylene-TCNQ complex: effects of chalcogen and fluorine substitutions DOI

Shubham Bajpai,

Raghu Nath Behera

Journal of Molecular Modeling, Journal Year: 2025, Volume and Issue: 31(2)

Published: Jan. 22, 2025

Language: Английский

Citations

0

Electrocrystallization of Copper 7,7,8,8‐Tetracyanoquinodimethane Charge‐Transfer Complex on Flexible Substrates for Real‐Time Ammonia Gas Sensing DOI Creative Commons
Ren Wang, Mohamed Kilani, Jiancheng Lin

et al.

Advanced Sensor Research, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 2, 2025

Abstract Real‐time monitoring of public safety, individual health, and environmental conditions relies on accurate continuous data collected by gas sensors, which provide users with cost‐effective insights to support informed decision‐making. This study presents an innovative approach that simplifies the manufacturing process nanowire (NW)‐based sensors enabling direct electrodeposition NW crystals various substrates, such as silicon wafers polyethylene terephthalate (PET). Copper 7,7,8,8‐Tetracyanoquinodimethane (CuTCNQ), a charge‐transfer complex, is electrodeposited directly onto photolithographically patterned interdigitated triangle‐tip electrodes functions chemiresistive sensor responds ammonia through charge interactions. The sensor's performance can be precisely controlled using electrochemical techniques, allowing for tailored sensitivity across different concentration ranges. To enhance practical application this technology, flexible, near‐field communication‐based passive tag developed integrating CuTCNQ flexible printed circuit board. device enables on‐demand analysis operates battery‐free wireless mobile phone scanning. capability crucial wearable or industrial devices aligns increasing demand robust solutions. represents significant step forward in improving both human health protection accessible efficient sensing technology.

Language: Английский

Citations

0

Topological and Optical properties of 2,7-Dichlorofluorescein Thin Films electrical characterization of Carbon/Dichlorofluorescein/p-Si/Al Photovoltaic devices DOI
Laila Almanqur

Optical Materials, Journal Year: 2025, Volume and Issue: unknown, P. 116731 - 116731

Published: Feb. 1, 2025

Language: Английский

Citations

0

Isoelectronic Push–Pull Fluorescent Difluoroborates: Halogen Bonding and Photophysical Properties DOI Creative Commons
Alex Iglesias-Reguant, Izabela Barańska, Damian Plażuk

et al.

The Journal of Organic Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 11, 2025

The structural and photophysical properties in the halogen bonding environment were thoroughly studied for a newly synthesized series of fluorescent dyes their model derivatives. analysis revealed that ground-state interactions among both are likewise. have push–pull topology, there is low-lying charge-transfer (CT) excited state electronic structure. In order to study effect intermolecular on parameters CT state, palette solvents was used (C6F6, C6F5Cl, C6F5Br, C6F5I). Our studies weak between perfluorohaloarene solvent heterocyclic core enhances states. results also demonstrated position nitrogen atom acceptor simultaneously controls directionality interaction influences emission wavelength fluorescence quantum yield. Experimental data further supported by quantum-chemical calculations. Overall, establishes direct link topology moiety prone specific probes.

Language: Английский

Citations

0

Electrically conductive charge-segregated pseudo-polymorphs comprising highly planar expanded π-electronic cation DOI Creative Commons
Yohei Haketa,

R. Nakajima,

Yuto Maruyama

et al.

Chemical Science, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Independently stacked positively and negatively charged π-electronic systems in charge-segregated columnar structures are desired for electronic properties derived from their electron-deficient -rich assembling states, respectively. An expanded cation, benzoporphyrin AuIII complex, was synthesized as the component of ion pairs combination with counteranions. In contrast to benzoporphyrin, which is known its insolubility organic solvents, bulky anions this study soluble common solvents. The formed assemblies two pseudo-polymorphs single-crystal less-crystalline (LeC) states based on stacking complex. XRD solid-state NMR measurements, along molecular dynamics (MD) simulation, revealed that LeC were by a less-ordered arrangement constituting ions induced electric conductivity observed assemblies.

Language: Английский

Citations

0

Photoresponsive Behavior of Triphenylamine‐Based Organic Small Molecule Emitters Involving a Photo‐Induced Charge‐Transfer Complexation Mechanism under UV Light DOI Open Access
Xiaoteng Jia, Yukun Yuan, Qi Lin

et al.

Chinese Journal of Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: March 20, 2025

Comprehensive Summary Stimuli‐responsive organic luminescent materials exhibit significant sensitivity to various external stimuli, among which their excellent photosensitivity is particularly prominent. This unique feature gives them great potential for applications. Herein, five small molecule emitters based on triphenylamine derivatives have been synthesized via Suzuki‐coupling reaction. These molecules fluorescence properties with quantum yields ( Φ ) all reaching over 90%. When irradiated a 365 nm UV lamp, interesting photochromic phenomena occurred in chloroform solutions. phenomenon has studied intensively by UV‐vis absorption and spectroscopy, EPR measurements, density functional theory calculations, finally, the group was used as photoinitiation precursor electron donor, photo‐induced charge transfer complex (PCTC) initiated donor successfully constructed.

Language: Английский

Citations

0

Reversible color changing response of pyrenylated charge-transfer probes towards Hg2+: linker-driven modulation of sensitivity and selectivity DOI Creative Commons
Nilanjan Dey

RSC Advances, Journal Year: 2025, Volume and Issue: 15(13), P. 9587 - 9593

Published: Jan. 1, 2025

Two easily synthesizable prenylated charge transfer probes with a terminal pyridine unit were designed. The compounds differ based on the nature of spacer: rigid olefinic (1) and flexible hydrazo (2). Both show exclusive interaction Hg2+ ions, leading to changes in visible color. Experimental analyses showed that compound 1 outperformed 2 terms sensitivity (A/A 0 ∼ 13-fold vs. ∼2-fold) detection limit (1.2 ppm 5.8 ppm), attributed its linker enhanced binding affinity. Moreover, ratiometric responses (r > 0.99) excellent selectivity for demonstrated. This study highlights development robust, reusable, cost-effective tools mercury detection, thus addressing critical environmental health concerns associated contamination. Environmental robustness was validated across solvents, counter-ions, water mixtures, decreasing efficacy high-water-content systems owing solvation effects probe aggregation. Mechanistic studies confirmed nitrogen as primary coordination site reversible binding, enabling reuse. Practical applications explored using paper strips modified probes, which facilitated rapid, cost-effective, quantitative via image analysis.

Language: Английский

Citations

0