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Positive and negative signal and line shape in stimulated Raman spectroscopy: Resonance femtosecond Raman spectra of diphenylbutadieneстатья
Статья опубликована в высокорейтинговом журнале
Информация о цитировании статьи получена из
Web of Science,
Scopus
Статья опубликована в журнале из списка Web of Science и/или Scopus
Дата последнего поиска статьи во внешних источниках: 11 апреля 2022 г.
- Авторы: Dobryakov A.L., Krohn O.A., Quick M., Ioffe I.N., Kovalenko S.A.
- Журнал: Journal of Chemical Physics
- Том: 156
- Номер: 8
- Год издания: 2022
- Издательство: AIP Publishing
- Местоположение издательства: United States
- Номер статьи: 084304
- DOI: 10.1063/5.0075116
- Аннотация: Resonance stimulated Raman signal and line shape are evaluated analytically under common electronic/vibrational dephasing and exponential Raman/probe pulse, exp(−|t|/τ). Generally, the signal from a particular state includes contributions from higher and lower electronic states. Thus, with S0 → S1 actinic excitation, the Raman signal consists of 15 Feynman diagrams entering with different signs. The negative sign indicates vibrational coherences in S1 or higher Sn, whereas the positive sign reveals coherences in S0 or Sn via S1 → Sn → Sm (n < m) coupling. The signal complexity is in contrast to spontaneous Raman with its single diagram only. The results are applied to femtosecond stimulated Raman spectra of trans–trans, cis–trans (ct), and cis–cis (cc) 1,4-diphenyl-1,3-butadiene, the ct and cc being reported for the first time. Upon actinic excitation, the Stokes spectra show negative bands from S1 or Sn. When approaching higher resonances Sn → Sm, some Raman bands switch their sign from negative to positive, thus, indicating new coherences in Sn. The results are discussed, and the measured Raman spectra are compared to the computed quantum-chemical spectra.
- Добавил в систему: Иоффе Илья Нафтольевич