دورية أكاديمية
Intramolecular Charge Transfer and Ultrafast Nonradiative Decay in DNA-Tethered Asymmetric Nitro- and Dimethylamino-Substituted Squaraines.
| العنوان: | Intramolecular Charge Transfer and Ultrafast Nonradiative Decay in DNA-Tethered Asymmetric Nitro- and Dimethylamino-Substituted Squaraines. |
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| المؤلفون: | Wright ND, Huff JS, Barclay MS, Wilson CK, Barcenas G, Duncan KM, Ketteridge M, Obukhova OM; SSI 'Institute for Single Crystals' of the National Academy of Sciences of Ukraine, Kharkiv 61072, Ukraine., Krivoshey AI; SSI 'Institute for Single Crystals' of the National Academy of Sciences of Ukraine, Kharkiv 61072, Ukraine., Tatarets AL; SSI 'Institute for Single Crystals' of the National Academy of Sciences of Ukraine, Kharkiv 61072, Ukraine., Terpetschnig EA; SETA BioMedicals, Urbana, Illinois 61801, United States., Dean JC; Department of Physical Science, Southern Utah University, Cedar City, Utah 84720, United States., Knowlton WB, Yurke B, Li L; Center for Advanced Energy Studies, Idaho Falls, Idaho 83401, United States., Mass OA, Davis PH; Center for Advanced Energy Studies, Idaho Falls, Idaho 83401, United States., Lee J, Turner DB, Pensack RD |
| المصدر: | The journal of physical chemistry. A [J Phys Chem A] 2023 Feb 09; Vol. 127 (5), pp. 1141-1157. Date of Electronic Publication: 2023 Jan 27. |
| نوع المنشور: | Journal Article |
| اللغة: | English |
| بيانات الدورية: | Publisher: American Chemical Society Country of Publication: United States NLM ID: 9890903 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1520-5215 (Electronic) Linking ISSN: 10895639 NLM ISO Abbreviation: J Phys Chem A Subsets: PubMed not MEDLINE; MEDLINE |
| أسماء مطبوعة: | Original Publication: Washington, D.C. : American Chemical Society, c1997- |
| مستخلص: | Molecular (dye) aggregates are a materials platform of interest in light harvesting, organic optoelectronics, and nanoscale computing, including quantum information science (QIS). Strong excitonic interactions between dyes are key to their use in QIS; critically, properties of the individual dyes govern the extent of these interactions. In this work, the electronic structure and excited-state dynamics of a series of indolenine-based squaraine dyes incorporating dimethylamino (electron donating) and/or nitro (electron withdrawing) substituents, so-called asymmetric dyes, were characterized. The dyes were covalently tethered to DNA Holliday junctions to suppress aggregation and permit characterization of their monomer photophysics. A combination of density functional theory and steady-state absorption spectroscopy shows that the difference static dipole moment (Δ d ) successively increases with the addition of these substituents while simultaneously maintaining a large transition dipole moment (μ). Steady-state fluorescence and time-resolved absorption and fluorescence spectroscopies uncover a significant nonradiative decay pathway in the asymmetrically substituted dyes that drastically reduces their excited-state lifetime (τ). This work indicates that Δ d can indeed be increased by functionalizing dyes with electron donating and withdrawing substituents and that, in certain classes of dyes such as these asymmetric squaraines, strategies may be needed to ensure long τ, e.g., by rigidifying the π-conjugated network. |
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| تواريخ الأحداث: | Date Created: 20230127 Date Completed: 20230209 Latest Revision: 20230215 |
| رمز التحديث: | 20230215 |
| مُعرف محوري في PubMed: | PMC9923757 |
| DOI: | 10.1021/acs.jpca.2c06442 |
| PMID: | 36705555 |
| قاعدة البيانات: | MEDLINE |
Find this issue from the American Chemical Society | تدمد: | 1520-5215 |
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| DOI: | 10.1021/acs.jpca.2c06442 |