利用飞秒自适应脉冲整形相干控制技术成功实现了甲醇溶液中甲基对称(vs(CH3)2832cm^-1)和反对称(vAS(CH3)2948cm^-1)振动能级相干反斯托克斯拉曼光谱(CARS)的选择激发。为了进一步探究双光束飞秒CARS光谱实现选择激发的机制,采用二次谐波频率分辨光学开关(SHG—FROG)测量方法对整形前后的泵浦激光脉冲进行了探测。SHG-FROG痕迹结果显示裁剪泵浦光中的有效频段可实现飞秒CARS的选择激发。研究表明飞秒自适应脉冲整形相干控制技术对于复杂分子系统飞秒CARS的选择激发研究具有非常重要的科学意义。
The selective excitation of coherent anti-Stokes Raman scattering (CARS) to the vs(CH3) (2832 cm^-1) and the vAs(CH3) (2948 cm^-1)vibrational modes from methanol solution is successfully achieved by adaptive femtosecond pulse shaping coherent control technology. In order to explore the mecha- nism of mode-selective excitation from two-pulse femtosecond CARS spectrum, second harmonic generation frequency-resolved optical gating (SHG-FROG) method is used to measure the original and optimal pump pulses. SHG-FROG traces indicate that the mode-selective excitation of femtosecond CARS spectrum can be achieved by manipulating the effective frequency components of the pump pulse related to specific molecular vibrational mode. The experimental results demonstrate that adaptive femtosecond pulse shaping coherent control technology has scientific significance for the complicated molecular systems.