Department of Chemical Sciences, University of Padova, Padova, Italy.
Phys Chem Chem Phys. 2013 Aug 21;15(31):12971-6. doi: 10.1039/c3cp51257f.
Multiphoton absorptions are important non-linear optical processes which allow us to explore excited states with low energy photons giving rise to new possibilities for photoinduced processes. Among these processes, multiphoton absorptions from excited states are particularly interesting because of the large susceptibilities characteristic of excited states. Here we explore the nonlinear transmission measurements recorded with 9 ns laser pulses at 1064 nm of the radical cations of (2-ferrocenyl)indene and of (2-ferrocenyl)-hexamethylindene, two interesting very stable molecules. The non-linear transmission data can be interpreted with a multiphoton sequence of three photon absorptions, the first being a one photon absorption related to the intramolecular charge transfer and the second a two photon absorption from the excited state created with the first process. The two photon absorption cross section is found to be several orders of magnitude larger than those usually found for two photon absorbing systems excited from the ground state.
多光子吸收是重要的非线性光学过程,它允许我们用低能量光子探测激发态,从而为光诱导过程带来新的可能性。在这些过程中,来自激发态的多光子吸收特别有趣,因为激发态的特性是大的极化率。在这里,我们研究了用 1064nm 的 9ns 激光脉冲记录的(2-二茂铁基)茚和(2-二茂铁基)-六甲基茚的自由基阳离子的非线性透射测量结果,这是两种非常稳定的有趣分子。非线性透射数据可以用三光子吸收的多光子序列来解释,第一个是与分子内电荷转移有关的单光子吸收,第二个是用第一个过程从激发态产生的双光子吸收。双光子吸收截面比通常从基态激发的双光子吸收系统大几个数量级。