دورية أكاديمية
Striking the right balance of intermolecular coupling for high-efficiency singlet fission.
| العنوان: | Striking the right balance of intermolecular coupling for high-efficiency singlet fission. |
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| المؤلفون: | Pensack RD; Department of Chemistry , Princeton University , Princeton , New Jersey 08544 , USA . Email: gscholes@princeton.edu., Tilley AJ; Department of Chemistry , University of Toronto , Toronto , Ontario M5S 3H6 , Canada., Grieco C; Department of Chemistry , The Pennsylvania State University , University Park , Pennsylvania 16802 , USA., Purdum GE; Department of Chemical and Biological Engineering , Princeton University , Princeton , New Jersey 08544 , USA., Ostroumov EE; Department of Chemistry , Princeton University , Princeton , New Jersey 08544 , USA . Email: gscholes@princeton.edu., Granger DB; Department of Chemistry , University of Kentucky , Lexington , Kentucky 40506 , USA . Email: anthony@uky.edu., Oblinsky DG; Department of Chemistry , Princeton University , Princeton , New Jersey 08544 , USA . Email: gscholes@princeton.edu., Dean JC; Department of Chemistry , Princeton University , Princeton , New Jersey 08544 , USA . Email: gscholes@princeton.edu., Doucette GS; Department of Chemistry , The Pennsylvania State University , University Park , Pennsylvania 16802 , USA., Asbury JB; Department of Chemistry , The Pennsylvania State University , University Park , Pennsylvania 16802 , USA., Loo YL; Department of Chemical and Biological Engineering , Princeton University , Princeton , New Jersey 08544 , USA.; Andlinger Center for Energy and the Environment , Princeton University , Princeton , New Jersey 08544 , USA., Seferos DS; Department of Chemistry , University of Toronto , Toronto , Ontario M5S 3H6 , Canada.; Department of Chemical Engineering and Applied Chemistry , University of Toronto , Toronto , Ontario M5S 3E5 , Canada., Anthony JE; Department of Chemistry , University of Kentucky , Lexington , Kentucky 40506 , USA . Email: anthony@uky.edu., Scholes GD; Department of Chemistry , Princeton University , Princeton , New Jersey 08544 , USA . Email: gscholes@princeton.edu. |
| المصدر: | Chemical science [Chem Sci] 2018 Jun 01; Vol. 9 (29), pp. 6240-6259. Date of Electronic Publication: 2018 Jun 01 (Print Publication: 2018). |
| نوع المنشور: | Journal Article |
| اللغة: | English |
| بيانات الدورية: | Publisher: Royal Society of Chemistry Country of Publication: England NLM ID: 101545951 Publication Model: eCollection Cited Medium: Print ISSN: 2041-6520 (Print) Linking ISSN: 20416520 NLM ISO Abbreviation: Chem Sci Subsets: PubMed not MEDLINE |
| أسماء مطبوعة: | Original Publication: Cambridge, UK : Royal Society of Chemistry, [2010]- |
| مستخلص: | Singlet fission is a process that splits collective excitations, or excitons, into two with unity efficiency. This exciton splitting process, unique to molecular photophysics, has the potential to considerably improve the efficiency of optoelectronic devices through more efficient light harvesting. While the first step of singlet fission has been characterized in great detail, subsequent steps critical to achieving overall highly-efficient singlet-to-triplet conversion are only just beginning to become well understood. One of the most elementary suggestions, which has yet to be tested, is that an appropriately balanced coupling is necessary to ensure overall highly efficient singlet fission; that is, the coupling needs to be strong enough so that the first step is fast and efficient, yet weak enough to ensure the independent behavior of the resultant triplets. In this work, we show how high overall singlet-to-triplet conversion efficiencies can be achieved in singlet fission by ensuring that the triplets comprising the triplet pair behave as independently as possible. We show that side chain sterics govern local packing in amorphous pentacene derivative nanoparticles, and that this in turn controls both the rate at which triplet pairs form and the rate at which they decay. We show how compact side chains and stronger couplings promote a triplet pair that effectively couples to the ground state, whereas bulkier side chains promote a triplet pair that appears more like two independent and long-lived triplet excitations. Our results show that the triplet pair is not emissive, that its decay is best viewed as internal conversion rather than triplet-triplet annihilation, and perhaps most critically that, in contrast to a number of recent suggestions, the triplets comprising the initially formed triplet pair cannot be considered independently. This work represents a significant step toward better understanding intermediates in singlet fission, and how molecular packing and couplings govern overall triplet yields. |
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| تواريخ الأحداث: | Date Created: 20180810 Latest Revision: 20231103 |
| رمز التحديث: | 20231215 |
| مُعرف محوري في PubMed: | PMC6062843 |
| DOI: | 10.1039/c8sc00293b |
| PMID: | 30090312 |
| قاعدة البيانات: | MEDLINE |
Full Text Finder | تدمد: | 2041-6520 |
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| DOI: | 10.1039/c8sc00293b |