Minimizing non-radiative decay in molecular aggregates through optimal control of excitonic coupling

Wang, Yuanheng; Ren, Jiajun; Shuai, Zhigang

doi:10.26434/chemrxiv-2022-q0w1l

Cited by 5 publications

(5 citation statements)

References 44 publications

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“…10 cm -1 , predominantly arising from the torsion of the spiroacridan-analogous moiety, contributes the most to the S j . The total reorganization energy (λ) of BN-Gefolded (675.8 cm -1 ) is found to be much lower than those of BN-C-folded and BN-Si-folded (1850.8 cm -1 and 3899.6 cm -1 respectively), leading to a relatively small k nr that is two orders of magnitude lower than the C and Si analogs, as λ is the dominant contributor of nonradiative decay 35,36 . The signi cant reduction in λ of BN-Ge-folded is probably due to the increased molecular rigidity [37][38][39] arising from the stronger π−π interaction.…”

Section: Theoretical Investigationsmentioning

confidence: 89%

Luminescent Organogermane Emitter with Folded Conformation for Operationally Stable Blue Organic Light-Emitting Diode

Tang,

Li,

Tang

et al. 2024

Preprint

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The exploration of heavy atom effect in organic semiconductors for organic light-emitting diode (OLED) applications has attracted much attention recently. While such effect has been extensively investigated in those incorporated with selenium, copper, silver and gold, there are only few studies on the role of germanium (Ge) on the luminescence and structural properties of emitters. Herein, we reveal the importance of the incorporation of Ge in multi-resonance thermally activated delayed fluorescence emitters that show improved luminescence properties than its carbon and silicon counterparts. We present the distinct single crystal structures of the two conformers of the organogermane emitter that co-exist in the solid state. We describe their conformational changes from open to folded geometries upon thermal stimulation under vacuum, as supported by variable-temperature single crystal diffraction analysis and theoretical calculations. From molecular dynamics simulations, we show that the folded form prevents a close proximity to the sensitizer in solid-state packing, thereby reducing Dexter energy transfer and facilitating efficient Förster energy transfer. Together with the spin-vibronic coupling and heavy atom effect, organogermane emitter shows an accelerated spin-flip process than its carbon and silicon counterparts. Based on the Ge emitter, we achieve a blue emission peaking at 479 nm with a narrow spectral full-width-at-half-maximum of 25 nm and a maximum external quantum efficiency of 38.4%. More importantly, we report the LT90 (90% of the initial luminance at 1000 cd m-2) of 2.2 h for Ge-based OLEDs, unlocking the full potential of organogermane emitters for operationally stable OLEDs. We anticipate our study provides insights into the design of organogermane compounds for optoelectronics applications.

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Section: Theoretical Investigationsmentioning

confidence: 89%

Luminescent Organogermane Emitter with Folded Conformation for Operationally Stable Blue Organic Light-Emitting Diode

Tang,

Li,

Tang

et al. 2024

Preprint

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“…In H‐aggregates, the transition dipoles are aligned “side by side,” resulting in a blue shift in the spectra and complete suppression of the radiative decay rate. H‐aggregates typically exhibit more non‐radiative dissipation pathways, thereby demonstrating excellent PCE (Wang et al, 2023). In contrast, in J‐aggregates, the transition dipoles are aligned “head to tail,” resulting in a red shift in the spectra.…”

Section: Mechanism Of the Enhanced Photothermal Performance Of Dye Ag...mentioning

confidence: 99%

Aggregation‐enhanced photothermal therapy of organic dyes

Yang,

Ji,

Yin

2024

WIREs Nanomed Nanobiotechnol

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Photothermal therapy (PTT) represents a groundbreaking approach to targeted disease treatment by harnessing the conversion of light into heat. The efficacy of PTT heavily relies on the capabilities of photothermal agents (PTAs). Among PTAs, those based on organic dyes exhibit notable characteristics such as adjustable light absorption wavelengths, high extinction coefficients, and high compatibility in biological systems. However, a challenge associated with organic dye‐based PTAs lies in their efficiency in converting light into heat while maintaining stability. Manipulating dye aggregation is a key aspect in modulating non‐radiative decay pathways, aiming to augment heat generation. This review delves into various strategies aimed at improving photothermal performance through constructing aggregation. These strategies including protecting dyes from photodegradation, inhibiting non‐photothermal pathways, maintaining space within molecular aggregates, and introducing intermolecular photophysical processes. Overall, this review highlights the precision‐driven assembly of organic dyes as a promising frontier in enhancing PTT‐related applications.This article is categorized under: Therapeutic Approaches and Drug Discovery > Emerging Technologies Therapeutic Approaches and Drug Discovery > Nanomedicine for Oncologic Disease Diagnostic Tools > In Vivo Nanodiagnostics and Imaging

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“…[23][24][25][26][27][28] The use of matrix product operator (MPO) [29][30][31][32][33] as tensor network operators to act on the wavefunction in the MPS form has facilitated the simulation of a wide range of phonon quantum dynamics. 20,[34][35][36][37][38] The conventional MPO is designed to handle a sum of products (SOP) of one-body operators, such as position operators and second quantization operators. However, in practice, considering the situation where globally coupled multi-dimensional potential energy surface is fitted by SOP, we cannot avoid the problem such as overfitting and limited representability.…”

Section: Introductionmentioning

confidence: 99%

Encoding a Many-body Potential Energy Surface into a Grid-Based Matrix Product Operator

Hino,

Kurashige

2024

Preprint

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An efficient algorithm for compressing a given many-body potential energy surface (PES) of molecular systems into a grid-based matrix product operator (MPO) is proposed. The PES is once represented by a full-dimensional or truncated many-body expansion form, which is obtained by ab initio calculations at each grid mesh point, and then all terms in the expansion are compressed and merged into a single MPO while maintaining the bond dimension of the MPO as small as possible. It was shown that the ab initio PES of the H2CO was compressed by more than two orders of magnitude in the size of the site operators without loss of accuracy. By the use of the grid basis, the tensor rank of the site operators of the MPO is reduced from four to three due to the diagonal nature of the position-dependent operators on the grid basis, which significantly reduces the computational cost of the tensor contractions required in the real and imaginary time evolution of the matrix product state (MPS) wavefunctions with the grid-based MPO (Grid-MPO) Hamiltonian. Similar to other grid-based methods, the Grid-MPO is readily applicable to any kind of potentials of molecular systems if the values at the grid points are available. Using the Grid-MPO combined with the MPS, we calculated the time correlation function of the Eigen cation \eigen to predict the infrared (IR) spectrum and compared with the experimental and the previous theoretical study. The actual scaling with the size of systems was examined for the multidimensional Henon-Heiles Hamiltonian. It was shown that the calculations are considerably accelerated by the graphic processing unit (GPU) because the sizes of site operators were kept small and all tensors were able to be stored on the VRAM of a GPU.

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Minimizing non-radiative decay in molecular aggregates through optimal control of excitonic coupling

Cited by 5 publications

References 44 publications

Luminescent Organogermane Emitter with Folded Conformation for Operationally Stable Blue Organic Light-Emitting Diode

Luminescent Organogermane Emitter with Folded Conformation for Operationally Stable Blue Organic Light-Emitting Diode

Aggregation‐enhanced photothermal therapy of organic dyes

Encoding a Many-body Potential Energy Surface into a Grid-Based Matrix Product Operator

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