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


Ontology type: schema:ScholarlyArticle      Open Access: True


Article Info

DATE

2016-12-12

AUTHORS

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

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. More... »

PAGES

467-473

Identifiers

URI

http://scigraph.springernature.com/pub.10.1038/nmat4816

DOI

http://dx.doi.org/10.1038/nmat4816

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1000487759

PUBMED

https://www.ncbi.nlm.nih.gov/pubmed/27941808


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17 schema:description 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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24 schema:keywords active molecules
25 atoms
26 backbone
27 biological processes
28 carbon atoms
29 carbon specificity
30 changes
31 crossing resonance
32 dynamics
33 excitation
34 excited state wavefunctions
35 excited states
36 exploration
37 kinetics
38 large number
39 laser-excited muon pump–probe spin spectroscopy
40 level crossing resonance
41 levels
42 light-induced changes
43 mapping
44 mechanism
45 method
46 molecular excitation
47 molecular excited states
48 molecules
49 muon pump–probe spin spectroscopy
50 number
51 observed time-dependent light-induced changes
52 pathway
53 pentacene backbone
54 photochemical processes
55 photochemical reaction kinetics
56 photochemical reactions
57 photochemical reactivity
58 photochemistry
59 potential
60 presence
61 process
62 pump–probe spin spectroscopy
63 reaction
64 reaction kinetics
65 reactivity
66 resolution
67 resonance
68 results
69 rigorous exploration
70 sensitivity
71 single-carbon level
72 spatial resolution
73 specific carbon atoms
74 specificity
75 spectroscopy
76 spin spectroscopy
77 state
78 state wavefunction
79 technique
80 temporal mapping
81 time-dependent light-induced changes
82 wavefunctions
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