Temporal mapping of photochemical reactions and molecular excited states with carbon specificity

K. Wang; P. Murahari; K. Yokoyama; J. S. Lord; F. L. Pratt; J. He; L. Schulz; M. Willis; J. E. Anthony; N. A. Morley; L. Nuccio; A. Misquitta; D. J. Dunstan; K. Shimomura; I. Watanabe; S. Zhang; P. Heathcote; A. J. Drew

doi:10.1038/NMAT4816

Temporal mapping of photochemical reactions and molecular excited states with carbon specificity

K. Wang, P. Murahari, K. Yokoyama, J. S. Lord, F. L. Pratt, J. He, L. Schulz, M. Willis, J. E. Anthony, N. A. Morley, L. Nuccio, A. Misquitta, D. J. Dunstan, K. Shimomura, I. Watanabe, S. Zhang, P. Heathcote, A. J. Drew

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10 Scopus citations

Abstract

Photochemical reactions are essential to a large number of important industrial and biological processes. A method for monitoring photochemical reaction kinetics and the dynamics of molecular excitations with spatial resolution within the active molecule would allow a rigorous exploration of the pathway and mechanism of photophysical and photochemical processes. Here we demonstrate that laser-excited muon pump–probe spin spectroscopy (photo-μSR) can temporally and spatially map these processes with a spatial resolution at the single-carbon level in a molecule with a pentacene backbone. The observed time-dependent light-induced changes of an avoided level crossing resonance demonstrate that the photochemical reactivity of a specific carbon atom is modified as a result of the presence of the excited state wavefunction. This demonstrates the sensitivity and potential of this technique in probing molecular excitations and photochemistry.

Original language	English
Pages (from-to)	467-474
Number of pages	8
Journal	Nature Materials
Volume	16
Issue number	4
DOIs	https://doi.org/10.1038/NMAT4816
State	Published - 2017

Bibliographical note

Publisher Copyright:
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.

Funding

A.J.D. would like to acknowledge financial support from the European Research Council (MuSES project, proposal number 307593) and Sichuan University. All authors would like to acknowledge the scientific and technical support provided by the ISIS pulsed muon and neutron source.We would like to acknowledge Litron Lasers Ltd., as this work would not have been possible without their exceptional customer service and technical expertise. K.W. was funded by the Chinese Scholarship Council. P.M. was funded by Queen Mary University of London, under the Principal’s Studentship scheme.

Funders	Funder number
Sichuan University	307593

ASJC Scopus subject areas

General Chemistry
General Materials Science
Condensed Matter Physics
Mechanics of Materials
Mechanical Engineering

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Wang, K., Murahari, P., Yokoyama, K., Lord, J. S., Pratt, F. L., He, J., Schulz, L., Willis, M., Anthony, J. E., Morley, N. A., Nuccio, L., Misquitta, A., Dunstan, D. J., Shimomura, K., Watanabe, I., Zhang, S., Heathcote, P., & Drew, A. J. (2017). Temporal mapping of photochemical reactions and molecular excited states with carbon specificity. Nature Materials, 16(4), 467-474. https://doi.org/10.1038/NMAT4816

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abstract = "Photochemical reactions are essential to a large number of important industrial and biological processes. A method for monitoring photochemical reaction kinetics and the dynamics of molecular excitations with spatial resolution within the active molecule would allow a rigorous exploration of the pathway and mechanism of photophysical and photochemical processes. Here we demonstrate that laser-excited muon pump–probe spin spectroscopy (photo-μSR) can temporally and spatially map these processes with a spatial resolution at the single-carbon level in a molecule with a pentacene backbone. The observed time-dependent light-induced changes of an avoided level crossing resonance demonstrate that the photochemical reactivity of a specific carbon atom is modified as a result of the presence of the excited state wavefunction. This demonstrates the sensitivity and potential of this technique in probing molecular excitations and photochemistry.",

author = "K. Wang and P. Murahari and K. Yokoyama and Lord, {J. S.} and Pratt, {F. L.} and J. He and L. Schulz and M. Willis and Anthony, {J. E.} and Morley, {N. A.} and L. Nuccio and A. Misquitta and Dunstan, {D. J.} and K. Shimomura and I. Watanabe and S. Zhang and P. Heathcote and Drew, {A. J.}",

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Wang, K, Murahari, P, Yokoyama, K, Lord, JS, Pratt, FL, He, J, Schulz, L, Willis, M, Anthony, JE, Morley, NA, Nuccio, L, Misquitta, A, Dunstan, DJ, Shimomura, K, Watanabe, I, Zhang, S, Heathcote, P & Drew, AJ 2017, 'Temporal mapping of photochemical reactions and molecular excited states with carbon specificity', Nature Materials, vol. 16, no. 4, pp. 467-474. https://doi.org/10.1038/NMAT4816

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AU - Murahari, P.

AU - Yokoyama, K.

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AU - Pratt, F. L.

AU - He, J.

AU - Schulz, L.

AU - Willis, M.

AU - Anthony, J. E.

AU - Morley, N. A.

AU - Nuccio, L.

AU - Misquitta, A.

AU - Dunstan, D. J.

AU - Shimomura, K.

AU - Watanabe, I.

AU - Zhang, S.

AU - Heathcote, P.

AU - Drew, A. J.

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AB - Photochemical reactions are essential to a large number of important industrial and biological processes. A method for monitoring photochemical reaction kinetics and the dynamics of molecular excitations with spatial resolution within the active molecule would allow a rigorous exploration of the pathway and mechanism of photophysical and photochemical processes. Here we demonstrate that laser-excited muon pump–probe spin spectroscopy (photo-μSR) can temporally and spatially map these processes with a spatial resolution at the single-carbon level in a molecule with a pentacene backbone. The observed time-dependent light-induced changes of an avoided level crossing resonance demonstrate that the photochemical reactivity of a specific carbon atom is modified as a result of the presence of the excited state wavefunction. This demonstrates the sensitivity and potential of this technique in probing molecular excitations and photochemistry.

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Temporal mapping of photochemical reactions and molecular excited states with carbon specificity

Abstract

Bibliographical note

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ASJC Scopus subject areas

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