Disentangling the complexity of coupled vibrations by two-dimensional electronic-vibrational spectroscopy
Abstract We employ two-dimensional electronic-vibrational (2DEV) spectroscopy to study the coherent dynamics of coupled vibrational modes in an excitonically-coupled dimer model. The advantage of separating excitation and detection in different frequency regimes allows us to directly probe the elect...
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| Published in | Journal of physics. B, Atomic, molecular, and optical physics Vol. 56; no. 14; pp. 145001 - 145010 |
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| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
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28.07.2023
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| Abstract | Abstract
We employ two-dimensional electronic-vibrational (2DEV) spectroscopy to study the coherent dynamics of coupled vibrational modes in an excitonically-coupled dimer model. The advantage of separating excitation and detection in different frequency regimes allows us to directly probe the electronic and vibrational coherences in the time-evolved 2DEV spectra. The complexity of vibrational coherence of two coupled modes is directly revealed by cross peaks in the 2DEV spectra. With the help of the ensuing time traces, we can follow how the vibrational coherence changes over time in the monomer model and, subsequently, in the dimer model. We show that the complexity of two coupled vibrational modes and the interaction between electronic and vibrational coherences in molecular systems can be effectively disentangled using the 2DEV spectroscopy technique. |
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| AbstractList | Abstract
We employ two-dimensional electronic-vibrational (2DEV) spectroscopy to study the coherent dynamics of coupled vibrational modes in an excitonically-coupled dimer model. The advantage of separating excitation and detection in different frequency regimes allows us to directly probe the electronic and vibrational coherences in the time-evolved 2DEV spectra. The complexity of vibrational coherence of two coupled modes is directly revealed by cross peaks in the 2DEV spectra. With the help of the ensuing time traces, we can follow how the vibrational coherence changes over time in the monomer model and, subsequently, in the dimer model. We show that the complexity of two coupled vibrational modes and the interaction between electronic and vibrational coherences in molecular systems can be effectively disentangled using the 2DEV spectroscopy technique. |
| Author | Zhang, Xuanchao Liang, Xian-Ting Dwayne Miller, R J Thorwart, Michael Liu, Zihui Duan, Hong-Guang Jha, Ajay |
| Author_xml | – sequence: 1 givenname: Xuanchao orcidid: 0009-0004-4748-0192 surname: Zhang fullname: Zhang, Xuanchao organization: Ningbo University Department of Physics, School of Physical Science and Technology, Ningbo 315211, People’s Republic of China – sequence: 2 givenname: Zihui surname: Liu fullname: Liu, Zihui organization: Ningbo University Department of Physics, School of Physical Science and Technology, Ningbo 315211, People’s Republic of China – sequence: 3 givenname: Ajay orcidid: 0000-0002-4489-518X surname: Jha fullname: Jha, Ajay organization: Rutherford Appleton Laboratory Research Complex at Harwell, Didcot OX11 0QX, United Kingdom – sequence: 4 givenname: Xian-Ting orcidid: 0000-0002-9955-6708 surname: Liang fullname: Liang, Xian-Ting organization: Ningbo University Department of Physics, School of Physical Science and Technology, Ningbo 315211, People’s Republic of China – sequence: 5 givenname: Michael surname: Thorwart fullname: Thorwart, Michael organization: The Hamburg Center for Ultrafast Imaging , Luruper Chaussee 149, 22761 Hamburg, Germany – sequence: 6 givenname: R J surname: Dwayne Miller fullname: Dwayne Miller, R J organization: University of Toronto The Departments of Chemistry and Physics, 80 St. George Street, Toronto M5S 3H6, Canada – sequence: 7 givenname: Hong-Guang surname: Duan fullname: Duan, Hong-Guang organization: Ningbo University Department of Physics, School of Physical Science and Technology, Ningbo 315211, People’s Republic of China |
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We employ two-dimensional electronic-vibrational (2DEV) spectroscopy to study the coherent dynamics of coupled vibrational modes in an... |
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| SubjectTerms | electronic coherence two-dimensional electronic vibrational spectroscopy vibrational coherence |
| Title | Disentangling the complexity of coupled vibrations by two-dimensional electronic-vibrational spectroscopy |
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