Solvation-Dependent Excited-State Dynamics of Donor–Acceptor Molecules with Hybridized Local and Charge Transfer Character
| العنوان: | Solvation-Dependent Excited-State Dynamics of Donor–Acceptor Molecules with Hybridized Local and Charge Transfer Character |
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| المؤلفون: | Andong Xia, Min Tao, Wei Zhang, Xinmiao Niu, Jie Kong, Damir Aumiler, Silvije Vdović, Yuguang Ma, Dehua Hu |
| المصدر: | The Journal of Physical Chemistry C. 124:5574-5582 |
| بيانات النشر: | American Chemical Society (ACS), 2020. |
| سنة النشر: | 2020 |
| مصطلحات موضوعية: | Physics, Dynamics (mechanics), Solvation, Charge (physics), 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, General Energy, Character (mathematics), Donor acceptor molecules, Chemical physics, Excited state, donor-acceptor molecules, charge transfer, Physical and Theoretical Chemistry, 0210 nano-technology |
| الوصف: | Recently, an organic synthetic strategy based on hybridized local and charge transfer (HLCT) character has been attracting much attention because of its potential for designing high-efficiency organic light emitting diode materials. In this work, two novel molecules, N, N-diphenyl-4-phenol-(1-phenyl-1H-phenanthro[9, 10-d]imidazol-2-yl)biphenyl-4-amine (TPA-PPI-OH) and N, N-diphenyl-4′-(1-phenyl-1H-phenanthro[9, 10-d]-imidazol-2-yl)-[1, 1′-biphenyl]-4-amine (TPA-PPI), were investigated by quantum chemical calculations, steady-state spectroscopy, and femtosecond transient absorption spectroscopy (fs-TA) to explore the nature of HLCT. Computational results and steady-state spectra suggest that the lowest excited state is dominated by local excitation (LE) character in low-polar toluene (TOL), whereas the charge transfer (CT) character plays the main role in high-polar acetonitrile (ACN) for both TPA-PPI-OH and TPA-PPI. Relative to TPA-PPI, TPA-PPI-OH shows less sensitivity to solvent polarity with higher quantum yields because of the more planar geometric structure, fabricated by inserting an additional intramolecular hydrogen bond (H-bond) to enhance the inflexibility of the molecule. Ultrafast fs-TA clearly shows the conversion of excited states from LE to CT with the increase of solvent polarity. The stimulated emission is mainly from the Ledominated lowest excited state in low-polar TOL, whereas CT dominates the final relaxation process in high-polar ACN because of strong solvation. Furthermore, the excited states being dominated by LE and CT simultaneously in medium-polar tetrahydrofuran is observed, while the quick equilibrium LE ↔ CT is established just after a femtosecond pulse excitation, indicating the typical HLCT character. The excited state deactivation process of TPA-PPI-OH is faster than that of TPA-PPI, which is attributed to the higher proportion of the LE component and the additional vibrational decay paths induced by the H-bond in TPA-PPI-OH. The results herein offer a guidance to understand the solvent-modulated excited state deactivation mechanism of HLCT molecules. |
| تدمد: | 1932-7455 1932-7447 |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::d9e958f8c9c78f75627263db6242c5e7 https://doi.org/10.1021/acs.jpcc.0c00003 |
| حقوق: | CLOSED |
| رقم الأكسشن: | edsair.doi.dedup.....d9e958f8c9c78f75627263db6242c5e7 |
| قاعدة البيانات: | OpenAIRE |
Find this issue from the American Chemical Society | تدمد: | 19327455 19327447 |
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