Multifaceted Ultrafast Intramolecular Charge Transfer Dynamics of 4‑(Dimethylamino)benzonitrile (DMABN)
Intramolecular charge transfer (ICT) of DMABN has been the subject of extensive investigations. Through the measurements of highly time-resolved fluorescence spectra (TRFS) over the whole emission region, we have examined the ICT dynamics of DMABN in acetonitrile free from the solvation dynamics and...
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| Published in | The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Vol. 117; no. 2; pp. 370 - 377 |
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| Main Authors | , , |
| Format | Journal Article |
| Language | English |
| Published |
Washington, DC
American Chemical Society
17.01.2013
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| Subjects | |
| Online Access | Get full text |
| ISSN | 1089-5639 1520-5215 1520-5215 |
| DOI | 10.1021/jp310842z |
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| Abstract | Intramolecular charge transfer (ICT) of DMABN has been the subject of extensive investigations. Through the measurements of highly time-resolved fluorescence spectra (TRFS) over the whole emission region, we have examined the ICT dynamics of DMABN in acetonitrile free from the solvation dynamics and vibronic relaxation. The ICT dynamics was found to be characterized by a broad range of time scales; nearly instantaneous (<30 fs), 160 fs, and 3.3 ps. TRFS revealed that an ICT state with partially twisted geometry, ICT(P), is formed within a few hundred femtoseconds either directly from the initial photoexcited state or via the locally excited (LE) state. The ICT(P) state undergoes further relaxation along the intramolecular nuclear coordinate to reach the twisted ICT (TICT) state with the time constant of 4.8 ps. A conformational diversity along the rotation of the dimethylamino group was speculated to account for the observed diffusive dynamics. |
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| AbstractList | Intramolecular charge transfer (ICT) of DMABN has been the subject of extensive investigations. Through the measurements of highly time-resolved fluorescence spectra (TRFS) over the whole emission region, we have examined the ICT dynamics of DMABN in acetonitrile free from the solvation dynamics and vibronic relaxation. The ICT dynamics was found to be characterized by a broad range of time scales; nearly instantaneous (<30 fs), 160 fs, and 3.3 ps. TRFS revealed that an ICT state with partially twisted geometry, ICT(P), is formed within a few hundred femtoseconds either directly from the initial photoexcited state or via the locally excited (LE) state. The ICT(P) state undergoes further relaxation along the intramolecular nuclear coordinate to reach the twisted ICT (TICT) state with the time constant of 4.8 ps. A conformational diversity along the rotation of the dimethylamino group was speculated to account for the observed diffusive dynamics. Intramolecular charge transfer (ICT) of DMABN has been the subject of extensive investigations. Through the measurements of highly time-resolved fluorescence spectra (TRFS) over the whole emission region, we have examined the ICT dynamics of DMABN in acetonitrile free from the solvation dynamics and vibronic relaxation. The ICT dynamics was found to be characterized by a broad range of time scales; nearly instantaneous (<30 fs), 160 fs, and 3.3 ps. TRFS revealed that an ICT state with partially twisted geometry, ICT(P), is formed within a few hundred femtoseconds either directly from the initial photoexcited state or via the locally excited (LE) state. The ICT(P) state undergoes further relaxation along the intramolecular nuclear coordinate to reach the twisted ICT (TICT) state with the time constant of 4.8 ps. A conformational diversity along the rotation of the dimethylamino group was speculated to account for the observed diffusive dynamics.Intramolecular charge transfer (ICT) of DMABN has been the subject of extensive investigations. Through the measurements of highly time-resolved fluorescence spectra (TRFS) over the whole emission region, we have examined the ICT dynamics of DMABN in acetonitrile free from the solvation dynamics and vibronic relaxation. The ICT dynamics was found to be characterized by a broad range of time scales; nearly instantaneous (<30 fs), 160 fs, and 3.3 ps. TRFS revealed that an ICT state with partially twisted geometry, ICT(P), is formed within a few hundred femtoseconds either directly from the initial photoexcited state or via the locally excited (LE) state. The ICT(P) state undergoes further relaxation along the intramolecular nuclear coordinate to reach the twisted ICT (TICT) state with the time constant of 4.8 ps. A conformational diversity along the rotation of the dimethylamino group was speculated to account for the observed diffusive dynamics. |
| Author | Joo, Taiha Kim, Chul Hoon Park, Myeongkee |
| AuthorAffiliation | POSTECH Pohang University of Science and Technology (POSTECH) |
| AuthorAffiliation_xml | – name: Pohang University of Science and Technology (POSTECH) – name: POSTECH |
| Author_xml | – sequence: 1 givenname: Myeongkee surname: Park fullname: Park, Myeongkee – sequence: 2 givenname: Chul Hoon surname: Kim fullname: Kim, Chul Hoon – sequence: 3 givenname: Taiha surname: Joo fullname: Joo, Taiha email: thjoo@postech.ac.kr |
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| Keywords | Fluorescence spectrum Chemical solution Benzenic compound fs range Nitriles Excited states Intramolecular charge transfer Organic compounds Ultrafast process |
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| Snippet | Intramolecular charge transfer (ICT) of DMABN has been the subject of extensive investigations. Through the measurements of highly time-resolved fluorescence... |
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| SubjectTerms | Acetonitrile Atomic and molecular physics Charge transfer Diffusion Dynamics Exact sciences and technology Femtosecond Fluorescence and phosphorescence spectra Fluorescence and phosphorescence; radiationless transitions, quenching (intersystem crossing, internal conversion) Molecular properties and interactions with photons Physical chemistry Physics Solvation Spectral emissivity |
| Title | Multifaceted Ultrafast Intramolecular Charge Transfer Dynamics of 4‑(Dimethylamino)benzonitrile (DMABN) |
| URI | http://dx.doi.org/10.1021/jp310842z https://www.ncbi.nlm.nih.gov/pubmed/23249244 https://www.proquest.com/docview/1273626853 https://www.proquest.com/docview/1753523924 |
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