Direct Tracking Excited-State Intramolecular Charge Redistribution of Acceptor–Donor–Acceptor Molecule by Means of Femtosecond Stimulated Raman Spectroscopy

التفاصيل البيبلوغرافية
العنوان: Direct Tracking Excited-State Intramolecular Charge Redistribution of Acceptor–Donor–Acceptor Molecule by Means of Femtosecond Stimulated Raman Spectroscopy
المؤلفون: Guoxian Zhang, Jie Kong, Julian M. W. Chan, Andong Xia, Wenqi Xu, Xinmiao Niu, Wei Zhang, Weimin Liu
المصدر: The Journal of Physical Chemistry B. 125:4456-4464
بيانات النشر: American Chemical Society (ACS), 2021.
سنة النشر: 2021
مصطلحات موضوعية: Materials science, 010304 chemical physics, Solvation, 010402 general chemistry, 01 natural sciences, Acceptor, Molecular physics, 0104 chemical sciences, Surfaces, Coatings and Films, symbols.namesake, Excited state, Intramolecular force, 0103 physical sciences, Femtosecond, Ultrafast laser spectroscopy, Materials Chemistry, symbols, Physics::Chemical Physics, Physical and Theoretical Chemistry, Raman spectroscopy, Raman scattering
الوصف: Symmetric quadrupolar molecules generally exhibit apolar ground states and dipolar excited states in a polar environment, which is explained by the excited state evolution from initial charge delocalization over all molecules to localization on one branch of the molecules after a femtosecond pulse excitation. However, direct observation of excited-state charge redistribution (delocalization/localization) is hardly accessible. Here, the intramolecular charge delocalization/localization character of a newly synthesized acceptor-donor-acceptor molecule (ADA) has been intensively investigated by femtosecond stimulated Raman scattering (FSRS) together with femtosecond transient absorption (fs-TA) spectroscopy. By tracking the excited state Raman spectra of the specific alkynyl (-C≡C-) bonds at each branch of ADA, we found that the nature of the relaxed S1 state is strongly governed by solvent polarity: symmetric delocalized intramolecular charge transfer (ICT) characters occurred in apolar solvent, whereas the asymmetric localized ICT characters appeared in polar solvent because of solvation. The solvation dynamics of ADA extracted from fs-TA is consistent with the time constants obtained by FSRS, but the FSRS clearly tracks the excited state intramolecular charge transfer delocalization/localization.
تدمد: 1520-5207
1520-6106
URL الوصول: https://explore.openaire.eu/search/publication?articleId=doi_dedup___::3f933ad18baefe536df3e4d9dd4d653e
https://doi.org/10.1021/acs.jpcb.1c01742
حقوق: CLOSED
رقم الأكسشن: edsair.doi.dedup.....3f933ad18baefe536df3e4d9dd4d653e
قاعدة البيانات: OpenAIRE