皮秒脉冲整形用于一般非对称陀螺分子的强三维无场排列
Picosecond pulse-shaping for strong three-dimensional field-free alignment of generic asymmetric-top molecules
摘要：
将分子固定在空间是分子结构和动力学成像的关键步骤。在这里，我们展示了三维（3D）的原型不对称的顶部分子吲哚使用椭圆偏振，形状，非共振激光脉冲的无场对齐。使用宽带激光脉冲的基于空间光调制器（SLM）的脉冲整形器，使用极端线性啁啾和受控相位和振幅整形的组合来产生截断的激光脉冲。通过对H $^+$和C $^{2+}$碎片的速度图成像，检测到了角约束效应。所实现的三维对准的特征在于将对准激光脉冲期间和之后的不同对准方向和不同时间的离子速度图测量结果与精确的计算结果进行比较。所实现的$\langle \cos^{2}δ\rangle=0.89$的强三维无场排列证明了通用复杂分子的强三维排列及其定量表征的可行性。
英文摘要：
Fixing molecules in space is a crucial step for the imaging of molecular structure and dynamics. Here, we demonstrate three-dimensional (3D) field-free alignment of the prototypical asymmetric top molecule indole using elliptically polarized, shaped, off-resonant laser pulses. A truncated laser pulse is produced using a combination of extreme linear chirping and controlled phase and amplitude shaping using a spatial-light-modulator (SLM) based pulse shaper of a broadband laser pulse. The angular confinement is detected through velocity-map imaging of H$^+$ and C$^{2+}$ fragments resulting from strong-field ionization and Coulomb explosion of the aligned molecules by intense femtosecond laser pulses. The achieved three-dimensional alignment is characterized by comparing the result of ion-velocity-map measurements for different alignment directions and for different times during and after the alignment laser pulse to accurate computational results. The achieved strong three-dimensional field-free alignment of $\langle \cos^{2}δ\rangle=0.89$ demonstrates the feasibility of both, strong three-dimensional alignment of generic complex molecules and its quantitative characterization.
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