Nonorthogonal Configuration Interaction for Singlet Fission: Beyond the Dimer

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

Published: Feb. 17, 2025

Language: Английский

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Modeling the Photophysical Processes of Organic Molecular Aggregates with Inclusion of Intermolecular Interactions and Vibronic Couplings

Published: May 17, 2024

Language: Английский

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Configuration Interaction in Frontier Molecular Orbital Basis for Screening the Spin-Correlated, Spatially Separated Triplet Pair State ¹(T···T) Formation

Journal of Chemical Theory and Computation, Journal Year: 2024, Volume and Issue: 20(19), P. 8624 - 8633

Published: Sept. 18, 2024

In the theoretical screening of Singlet Fission rates in molecular aggregates, often frontier orbital model for dimers is employed. However, dimer approach fails to account recent experimental findings that suggest singlet fission progresses through a further intermediate state featuring two spatially separated, spin-correlated triplets, specifically

Language: Английский

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Identification of the interchromophore interaction in the electronic absorption and circular dichroism spectra of bis-phenanthrenes

Physical Chemistry Chemical Physics, Journal Year: 2024, Volume and Issue: 26(7), P. 6155 - 6163

Published: Jan. 1, 2024

This work aims to identify the contribution of different types excited states electronic absorption and ECD spectra unveil character low-lying states.

Language: Английский

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Singlet Fission in Diphenylhexatriene Amide Derivatives: Effects of Intermolecular Hydrogen Bonds in Crystals

The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: 128(20), P. 8277 - 8287

Published: May 13, 2024

Singlet fission (SF) is a photophysical process where one high-energy singlet exciton (S*) interacts with an adjacent ground-state molecule to produce two low-energy triplet excitons (T) via correlated pair [(TT)]. As exciton-multiplication process, SF can potentially increase the photon-to-electricity conversion efficiency of solar cells and optoelectronic devices. In organic materials, depends strongly on E(S*)/E(T) energetics extent electronic coupling between interacting molecules. Strong intermolecular interactions such as hydrogen bonds are often effectively utilized control molecular arrangement in crystals; however, our understanding effects solid-state still insufficient. Here, we investigate kinetics series newly synthesized 1,6-diphenyl-1,3,5-hexatriene (DPH) derivatives amide [CONHR (R = Me, Et, Pr, Bu) NHCOMe] ring substituents. Crystallographic FT-IR spectral analyses confirm presence NH···O═C resulting close proximity Fluorescence decay measurements analysis reveal that S* → (TT) rates not very different for amides unsubstituted hydrocarbon DPH, while T + clearly faster than DPH. Considering similar all trienes, acceleration be attributed enhanced crystals.

Language: Английский

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Artificial Intelligence Warm-Start Approach: Optimizing the Generalization Capability of QAOA in Complex Energy Landscapes

New Journal of Physics, Journal Year: 2024, Volume and Issue: 26(5), P. 053016 - 053016

Published: May 1, 2024

Abstract To address the issue of quantum approximate optimization algorithm frequently encountering local minima and cost parameter within complex non-convex energy landscapes, we consider a warm-start method. This approach leverages characteristics transition states in enhanced optimizer, specifically descending along unique negative curvature directions, to find smaller minima. Our research results indicate that with assistance an pre-training structure AlphaZero AI model, initialization generalization ability new optimizer is significantly across various test sets. We train on 2-SAT training sets clause densities between α ≈ 2.6 2.89, transfer more Additionally, average residual density learning consistently remains below 0.01, even achieving high success probability 98% hard instances 3.7. The search efficiency, pre-trained by ensemble learning, was enhanced, while only requiring simple interpolation few points global optimal solutions at higher sample densities.

Language: Английский

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Electronic Absorption and Circular Dichroism Spectra of One-Dimensional Bay-Substituted Chiral PDIs: Effects of Intermolecular Interactions, Vibronic Coupling, and Aggregate Size

The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: 128(47), P. 20253 - 20263

Published: Nov. 13, 2024

Electronic circular dichroism (ECD) spectroscopy is the preferred tool for studying organic chiral supramolecules. However, it a great challenge to experimentally clarify contributions ECD spectra from molecular vibrational motions and intermolecular interactions, key factors an efficient system architecture design of chemical sensors, catalysts, or optoelectronics. Focusing on this issue, here, we perform theoretical studies vibrationally resolved absorption two one-dimensional bay-substituted perylene diimides (PDIs) by employing non-Markovian stochastic Schrödinger equation (NMSSE) with respect model Hamiltonian in diabatic representation, which includes intramolecular localized excited states (LEs), change-transfer (CTEs), vibronic couplings (VC) as well. Our calculated results exhibit that spectra, inclusion VC effect, agree better experimental ones than those without effect difference between traditional PDIs much less obvious their verifying sensitive absolute configuration conformation We further make comparison among pure electronic aggregates different aggregate sizes time-dependent density functional theory mixed exciton decoupling LE CTE states. It shown hybridization emergence new peaks troughs high-energy band significant deviation spectrum predicted chirality rule. oligomers odd–even alternation pattern changes size.

Language: Английский

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Comment on “A posteriori localization of many‐body excited states through simultaneous diagonalization”

Journal of Computational Chemistry, Journal Year: 2023, Volume and Issue: 44(27), P. 2158 - 2159

Published: July 15, 2023

We comment on an excited-state localization method recently proposed by Blanc et al. (J. Comput. Chem. 2023, 44, 105). Elaborate comparisons are made to demonstrate that their is a less-comprehensive version of the diabatization us 2 years earlier Phys. Lett. 2021, 12, 1032).

Language: Английский

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