Revealing ultrafast vibronic dynamics of tetracene molecules with sub-8 fs UV impulsive Raman spectroscopy

Teramoto, Takahiro; Liu, Jun; Du, Juan; Kobayashi, Takayoshi

doi:https://doi.org/10.1039/d2cp03572c

Revealing ultrafast vibronic dynamics of tetracene molecules with sub-8 fs UV impulsive Raman spectroscopy

Teramoto, Takahiro; Liu, Jun; Du, Juan et al.

Physical Chemistry Chemical Physics, 2022, 24(45), 27783-27792

アクセス数:509件（2026-07-26 22:40 集計）

固定URL: https://hdl.handle.net/11094/89743

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タイトル	Revealing ultrafast vibronic dynamics of tetracene molecules with sub-8 fs UV impulsive Raman spectroscopy
著者	NRID 1000040467056 1000040467056 researchmap permalink read0139851 read0139851 Scopus Author ID 56679221100 56679221100 著者名 Teramoto, Takahiro
	著者名 Liu, Jun
	著者名 Du, Juan
	著者名 Kobayashi, Takayoshi
抄録	Ultrafast dynamics of tetracene molecules in THF solution were investigated using sub-8 fs ultraviolet pulse lasers and ab initio calculations. The time trace of absorbance changes exhibited ultrafast decay with a time constant of 165 ± 10 fs because of the relaxation from a vibronically hot excited state to the potential minimum in the S1 state. From the signals of absorbance changes in the negative time region, we obtained the electronic dephasing time of 31.27 ± 1.63 fs. Inverse Fourier transform of stationary absorption spectra exhibited rapid decay with 2.1 ± 0.08 fs. From these data, we estimated the ratio of total dephasing time to homogenous and inhomogeneous broadening as 6.7% and 93.3%, respectively. Impulsive Raman spectra reflect the wave packet dynamics of vibrational modes. Although inhomogeneous broadening blurred the phase jump across the resonance peak in the spectral range, 1156 and 1680 cm−1 vibrational modes exhibited a phase jump from −π to ∼π and −0.5π to ∼0.5π, respectively. The amplitude profiles of these vibrational modes agree with simulated vibronic progressions of combination bands. Time-frequency analysis revealed coupling dynamics between low- and high-frequency modes, where high-frequency modes are in-plane motions and low-frequency modes are out-of-plane motions. Therefore, these coupling dynamics induce symmetry-breaking of the molecular framework, which fastens the singlet fission process.
出版者	Royal Society of Chemistry
収録物名	Physical Chemistry Chemical Physics
巻(号)	24(45)
ページ	27783-27792
刊行年月	2022-11-02
言語	英語
ハンドルURL	https://hdl.handle.net/11094/89743
PISSN	14639076
NCID	AA11301773
関連情報 (isVersionOf)	DOI (出版社版) https://doi.org/10.1039/d2cp03572c
アクセス権	open access
権利情報	Reproduced from Phys. Chem. Chem. Phys., 2022, 24, 27783-27792 with permission from the Royal Society of Chemistry.
出版タイプ	Accepted Manuscript
カテゴリ	学術雑誌論文 Journal Article

資源タイプ	学術雑誌論文
ローカル資源タイプ	学術雑誌論文
DCMI資源タイプ	text
DCTERMS.bibliographicCitation	Physical Chemistry Chemical Physics. 2022, 24(45), p. 27783-27792
DC.title	Revealing ultrafast vibronic dynamics of tetracene molecules with sub-8 fs UV impulsive Raman spectroscopy
DC.creator	Teramoto, Takahiro
	Liu, Jun
	Du, Juan
	Kobayashi, Takayoshi
DC.publisher	Royal Society of Chemistry
DC.language' scheme='DCTERMS.RFC1766	英語
DC.type' scheme='DCTERMS.DCMIType	text
DCTERMS.issued' scheme='DCTERMS.W3CDTF	2022-11-02
DC.identifier	https://doi.org/10.1039/d2cp03572c
DCTERMS.abstract	Ultrafast dynamics of tetracene molecules in THF solution were investigated using sub-8 fs ultraviolet pulse lasers and ab initio calculations. The time trace of absorbance changes exhibited ultrafast decay with a time constant of 165 ± 10 fs because of the relaxation from a vibronically hot excited state to the potential minimum in the S1 state. From the signals of absorbance changes in the negative time region, we obtained the electronic dephasing time of 31.27 ± 1.63 fs. Inverse Fourier transform of stationary absorption spectra exhibited rapid decay with 2.1 ± 0.08 fs. From these data, we estimated the ratio of total dephasing time to homogenous and inhomogeneous broadening as 6.7% and 93.3%, respectively. Impulsive Raman spectra reflect the wave packet dynamics of vibrational modes. Although inhomogeneous broadening blurred the phase jump across the resonance peak in the spectral range, 1156 and 1680 cm−1 vibrational modes exhibited a phase jump from −π to ∼π and −0.5π to ∼0.5π, respectively. The amplitude profiles of these vibrational modes agree with simulated vibronic progressions of combination bands. Time-frequency analysis revealed coupling dynamics between low- and high-frequency modes, where high-frequency modes are in-plane motions and low-frequency modes are out-of-plane motions. Therefore, these coupling dynamics induce symmetry-breaking of the molecular framework, which fastens the singlet fission process.
DC.rights	Reproduced from Phys. Chem. Chem. Phys., 2022, 24, 27783-27792 with permission from the Royal Society of Chemistry.
DC.format	89743
citation_title	Revealing ultrafast vibronic dynamics of tetracene molecules with sub-8 fs UV impulsive Raman spectroscopy
citation_author	Teramoto, Takahiro
	Liu, Jun
	Du, Juan
	Kobayashi, Takayoshi
citation_publisher	Royal Society of Chemistry
citation_language	英語
citation_date	2022-11-02
citation_journal_title	Physical Chemistry Chemical Physics
citation_volume	24
citation_issue	45
citation_firstpage	27783
citation_lastpage	27792
citation_doi	https://doi.org/10.1039/d2cp03572c
citation_public_url	https://hdl.handle.net/11094/89743

Revealing ultrafast vibronic dynamics of tetracene molecules with sub-8 fs UV impulsive Raman spectroscopy

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