Singlet exciton fission dynamics in 6,13-diphenylpentacene nanoaggregate and thin film

IF 4.7 2区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Molecular Structure Pub Date : 2025-07-15 Epub Date: 2025-03-01 DOI:10.1016/j.molstruc.2025.141921
Amitabha Nandi , Rajib Ghosh
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Abstract

Pentacene is the archetypal example of singlet fission material in polyacene family with fastest known singlet fission rate (τSF <100 fs). However, pentacene suffers from fast chemical and photochemical degradation in ambient condition, mainly by oxidation at 6 and 13-positon and hence limits prospects in optoelectronic application. Herein we show phenyl substituted pentacene at 6 and 13 position offers improved photo-stability with preserved SF property. Detailed transient pump-probe spectroscopic investigation on 6,13-diphenylpentacene (DPPn) thin film and nanoaggregates shows efficient singlet exciton fission process occurring in tens of picosecond timescale. In comparison to pentacene, though SF rate in DPPn is observed to slow down about two orders of magnitude due to weaker electronic coupling imposed by two phenyl substitution, triplet yield remains attractively high (∼ 180 %). Remarkably, thermal and photochemical stability of the DPPn thin film (remains stable over several months in ambient condition) is observed to be much superior than pentacene and thus proposed to be more useful for practical application in optoelectronic devices.

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6,13-二苯并五烯纳米聚集体与薄膜的单线态激子裂变动力学
并五苯是聚四苯族中单线态裂变材料的典型例子,已知单线态裂变速率最快(τSF <100 fs)。然而,并五苯在环境条件下的化学和光化学降解速度快,主要是在6位和13位氧化,因此限制了光电应用的前景。本研究表明,6位和13位的苯基取代并戊烯具有更好的光稳定性,并保留了SF特性。对6,13-二苯并五苯(DPPn)薄膜和纳米聚集体的瞬态泵探光谱研究表明,单线态激子裂变过程发生在几十皮秒的时间尺度上。与并五苯相比,虽然由于两个苯基取代所施加的电子耦合较弱,DPPn中的SF速率被观察到减慢了大约两个数量级,但三联体产率仍然很高(~ 180%)。值得注意的是,DPPn薄膜的热稳定性和光化学稳定性(在环境条件下保持数月稳定)比并五苯要好得多,因此被认为在光电器件的实际应用中更有用。
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来源期刊
Journal of Molecular Structure
Journal of Molecular Structure 化学-物理化学
CiteScore
7.10
自引率
15.80%
发文量
2384
审稿时长
45 days
期刊介绍: The Journal of Molecular Structure is dedicated to the publication of full-length articles and review papers, providing important new structural information on all types of chemical species including: • Stable and unstable molecules in all types of environments (vapour, molecular beam, liquid, solution, liquid crystal, solid state, matrix-isolated, surface-absorbed etc.) • Chemical intermediates • Molecules in excited states • Biological molecules • Polymers. The methods used may include any combination of spectroscopic and non-spectroscopic techniques, for example: • Infrared spectroscopy (mid, far, near) • Raman spectroscopy and non-linear Raman methods (CARS, etc.) • Electronic absorption spectroscopy • Optical rotatory dispersion and circular dichroism • Fluorescence and phosphorescence techniques • Electron spectroscopies (PES, XPS), EXAFS, etc. • Microwave spectroscopy • Electron diffraction • NMR and ESR spectroscopies • Mössbauer spectroscopy • X-ray crystallography • Charge Density Analyses • Computational Studies (supplementing experimental methods) We encourage publications combining theoretical and experimental approaches. The structural insights gained by the studies should be correlated with the properties, activity and/ or reactivity of the molecule under investigation and the relevance of this molecule and its implications should be discussed.
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