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典型文献
Laser control strategies in full-dimensional funneling dynamics:the case of pyrazine[Invited]
文献摘要:
Motivated by the major role funneling dynamics plays in light-harvesting processes,we built some laser control strategies inspired from basic mechanisms such as interference and kicks,and applied them to the case of pyrazine.We are studying the internal conversion between the two excited states,the highest and directly reachable from the initial ground state being considered as a donor and the lowest as an acceptor.The ultimate control objective is the maximum population deposit in the otherwise dark acceptor from a two-step process:radiative excitation of the donor,followed by a conical-intersection-mediated funneling towards the acceptor.The overall idea is to first obtain the control field param-eters[individual pulses leading frequency and intensity,duration,and inter-pulse time delay]for tractable reduced dimen-sional models basically describing the conical intersection branching space.Once these parameters are optimized,they are fixed and used in full-dimensional dynamics describing the electronic population transfer.In the case of pyrazine,the reduced model is four-dimensional,whereas the full dynamics involves 24 vibrational modes.Within experimentally achiev-able electromagnetic field requirements,we obtain a robust control with about 60%of the ground state population depos-ited in the acceptor state,while about 16%remains in the donor.Moreover,we anticipate a possible transposition to the control of even larger molecular systems,for which only a small number of normal modes are active,among all the others acting as spectators in the dynamics.
文献关键词:
作者姓名:
Samrit Mainali;Fabien Gatti;Osman Atabek
作者机构:
Institut des Sciences Moléculaires d'Orsay,CNRS,Université Paris-Saclay,91405 Orsay,France
引用格式:
[1]Samrit Mainali;Fabien Gatti;Osman Atabek-.Laser control strategies in full-dimensional funneling dynamics:the case of pyrazine[Invited])[J].中国光学快报(英文版),2022(10):30-41
A类:
funneling
B类:
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AB值:
0.564998
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