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

被引:0
|
作者
Wang, K. [1 ,2 ]
Murahari, P. [2 ]
Yokoyama, K. [2 ,3 ]
Lord, J. S. [3 ]
Pratt, F. L. [3 ]
He, J. [1 ]
Schulz, L. [1 ]
Willis, M. [1 ]
Anthony, J. E. [4 ]
Morley, N. A. [5 ]
Nuccio, L. [6 ,7 ]
Misquitta, A. [2 ]
Dunstan, D. J. [2 ]
Shimomura, K. [8 ]
Watanabe, I. [9 ]
Zhang, S. [1 ]
Heathcote, P. [10 ]
Drew, A. J. [1 ,2 ,3 ]
机构
[1] Sichuan Univ, Coll Phys Sci & Technol, Chengdu 610064, Sichuan, Peoples R China
[2] Queen Mary Univ London, Sch Phys & Astron, London E1 4NS, England
[3] Rutherford Appleton Lab, ISIS Muon Facil, Didcot OX11 0QX, Oxon, England
[4] Univ Kentucky, Dept Chem, Lexington, KY 40506 USA
[5] Univ Sheffield, Dept Mat Sci & Engn, Sheffield S1 3JD, S Yorkshire, England
[6] Univ Fribourg, Dept Phys, Chemin Musee 3, CH-1700 Fribourg, Switzerland
[7] Fribourg Ctr Nanomat, Chemin Musee 3, CH-1700 Fribourg, Switzerland
[8] J PARC Ctr, Mat & Life Sci Div, Tokai, Ibaraki 3191195, Japan
[9] RIKEN, RAL, Nishina Ctr, 2-1 Hirosawa, Wako, Saitama 3510198, Japan
[10] Queen Mary Univ London, Sch Biol & Chem Sci, London E1 4NS, England
基金
欧洲研究理事会;
关键词
LIGHT-EMITTING-DIODES; MUONIUM; FISSION; ULTRAVIOLET;
D O I
10.1038/NMAT4816
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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-mu SR) 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.
引用
收藏
页码:467 / +
页数:8
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