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  Transporting and concentrating vibrational energy to promote isomerization

Lau, J. A., Chen, L., Choudhury, A., Schwarzer, D., Verma, V. B., & Wodtke, A. M. (2021). Transporting and concentrating vibrational energy to promote isomerization. Nature, 589(7842), 391-395. doi:10.1038/s41586-020-03081-y.

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 Creators:
Lau, J. A.1, Author              
Chen, L.1, Author              
Choudhury, A.1, Author              
Schwarzer, D.1, Author              
Verma, V. B., Author
Wodtke, A. M.2, Author              
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1Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society, ou_578600              
2Department of Dynamics at Surfaces, MPI for biophysical chemistry, Max Planck Society, ou_578600              

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Free keywords: Chemical physics, Surface chemistry
 Abstract: Visible-light absorption and transport of the resultant electronic excitations to a reaction centre through Förster resonance energy transfer1,2,3 (FRET) are critical to the operation of biological light-harvesting systems4, and are used in various artificial systems made of synthetic dyes5, polymers6 or nanodots7,8. The fundamental equations describing FRET are similar to those describing vibration-to-vibration (V–V) energy transfer9, and suggest that transport and localization of vibrational energy should, in principle, also be possible. Although it is known that vibrational excitation can promote reactions10,11,12,13,14,15,16, transporting and concentrating vibrational energy has not yet been reported. We have recently demonstrated orientational isomerization enabled by vibrational energy pooling in a CO adsorbate layer on a NaCl(100) surface17. Here we build on that work to show that the isomerization reaction proceeds more efficiently with a thick 12C16O overlayer that absorbs more mid-infrared photons and transports the resultant vibrational excitations by V–V energy transfer to a 13C18O–NaCl interface. The vibrational energy density achieved at the interface is 30 times higher than that obtained with direct excitation of the interfacial CO. We anticipate that with careful system design, these concepts could be used to drive other chemical transformations, providing new approaches to condensed phase chemistry.

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Language(s): eng - English
 Dates: 2021-01-112021-01-21
 Publication Status: Published in print
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 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41586-020-03081-y
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Title: Nature
Source Genre: Journal
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Pages: - Volume / Issue: 589 (7842) Sequence Number: - Start / End Page: 391 - 395 Identifier: -