Academic Journal

Role of Singlet and Triplet Excited States in the Oxygen-Mediated Photophysics and Photodegradation of Polyacenes

التفاصيل البيبلوغرافية
العنوان: Role of Singlet and Triplet Excited States in the Oxygen-Mediated Photophysics and Photodegradation of Polyacenes
المؤلفون: Alexandra N. Stuart, Tak W. Kee, David M. Huang
سنة النشر: 2024
مصطلحات موضوعية: Biophysics, Biochemistry, Inorganic Chemistry, Biological Sciences not elsewhere classified, Chemical Sciences not elsewhere classified, Physical Sciences not elsewhere classified, increased photovoltaic efficiencies, common model systems, different excited states, triplet excited states, polyacene triplet population, oxygen degrade polyacenes, excited states, polyacenes polyacenes, triplet state, triplet fusion, resolved excited, excited singlet, world environments, world applications, unwanted endoperoxides, thus enhanced, state dynamics, significantly influence, predominant mechanism, photophysical phenomena, particular enhancing, molecule ’, may lead, generation photovoltaics
الوصف: Polyacenes, such as tetracene and pentacene, are common model systems for the study of photophysical phenomena such as singlet fission (SF) and triplet fusion, processes which may lead to increased photovoltaic efficiencies. While they exhibit desirable photophysical properties, these materials are not photostable and convert to unwanted endoperoxides in the presence of oxygen and light, limiting their use in real-world applications. Not only does oxygen degrade polyacenes but also it can affect their photophysics, leading to both the sensitization and quenching of different excited states. In this study, we characterize the effect of oxygen on 5,12-bis(triisopropylsilylethynyl) tetracene (TIPS-Tn) and 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS-Pn) using transient absorption spectroscopy, and show that oxygen can significantly influence the population of excited states, in particular enhancing the polyacene triplet population. We additionally combine the time-resolved excited-state dynamics with photodegradation studies to determine the predominant mechanism of photooxidation, which has previously been unclear. We find that both molecules photodegrade predominantly via singlet oxygen; however, for TIPS-Tn, this occurs through the triplet state, whereas for TIPS-Pn, degradation occurs through the excited singlet. The photodegradation of TIPS-Tn is thus enhanced by faster rates of SF, whereas SF in TIPS-Pn increases the molecule’s photostability. This work has implications both for the design of new materials for next-generation photovoltaics that can avoid photooxidation and for the study of their photophysics in real-world environments.
نوع الوثيقة: article in journal/newspaper
اللغة: unknown
Relation: https://figshare.com/articles/journal_contribution/Role_of_Singlet_and_Triplet_Excited_States_in_the_Oxygen-Mediated_Photophysics_and_Photodegradation_of_Polyacenes/24975266
DOI: 10.1021/jacs.3c12245.s001
الاتاحة: https://doi.org/10.1021/jacs.3c12245.s001
https://figshare.com/articles/journal_contribution/Role_of_Singlet_and_Triplet_Excited_States_in_the_Oxygen-Mediated_Photophysics_and_Photodegradation_of_Polyacenes/24975266
Rights: CC BY-NC 4.0
رقم الانضمام: edsbas.62C62EC3
قاعدة البيانات: BASE
الوصف
DOI:10.1021/jacs.3c12245.s001