Department of Physics and State Key Laboratory of Precision Spectroscopy, East China Normal University, 200062 Shanghai, People's Republic of China.
J Chem Phys. 2010 Mar 7;132(9):094503. doi: 10.1063/1.3327843.
Coherent control of two-photon fluorescence (TPF) of 2',7'-dichlorofluorescein in methanol solution was experimentally investigated by shaping the femtosecond pulse with the phase jump. The experimental results indicated that the TPF intensity induced by the shaped femtosecond pulses with certain phase jump could be coherently enhanced. The physical mechanisms for TPF enhancement in the molecular system were explicitly discussed and analyzed, which could be attributed to the wave-packet constructive interference in the excited states. Finally, two phase-locked femtosecond pulses were used to explore the wave-packet constructive interference in the excited states of 2',7'-dichlorofluorescein, which validate experimentally the proposed mechanism.
实验研究了通过相位跃变对飞秒脉冲整形来实现甲醇溶液中 2',7'-二氯荧光素的双光子荧光（TPF）的相干控制。实验结果表明，具有一定相位跃变的飞秒脉冲诱导的 TPF 强度可以相干增强。明确讨论和分析了分子体系中 TPF 增强的物理机制，这归因于激发态中的波包相干干涉。最后，使用两个锁相飞秒脉冲来研究 2',7'-二氯荧光素激发态中的波包相干干涉，实验验证了所提出的机制。
