双光子计算公式的审稿意见求助

小苹果gugu

各位老师好，我投稿了一篇有关PET机理的双光子的文章，收到一条审稿意见：In equation, the authors are using a perturbated description of the two photon process. This methodology requires that there is no states at the one-photon energy (probably true) and strongly changes with the number of states in the expansion. Did the authors check the convergence with the number of states in the expansion? Moreover, since the states are calculated with TD-DFT (probably in the TDA approximation), the expansion is restricted to singles excitations. This approximation is reasonable for one-photon transitions but can be problematic for TPA since the transition can go to a double excited state not described at TD-DFT. Is there any study using ab initio methodology for a similar chromophore to discard this problem?按照前人的研究，都是使用该公式进行计算的，审稿人提出的问题我不是很能理解，我已经在dalton软件中计算了6，8，10，12，14个态的双光子，求助各位老师，我应该如何回复审稿人，谢谢各位老师。

wzkchem5

第一个问题，把你做了不同数目的态的计算结果对态数作图，外推到无穷多个态，证明外推结果和14个态的计算结果之差可以忽略
第二个问题，查研究类似体系且考虑了双激发态（注意不是双光子吸收，是涉及两个电子同时跃迁的激发态）的文献，引文献结论证明双激发态的贡献可以忽略

小苹果gugu

wzkchem5 发表于 2023-4-20 16:09
第一个问题，把你做了不同数目的态的计算结果对态数作图，外推到无穷多个态，证明外推结果和14个态的计算结 ...

谢谢老师的专业解答~