Miyabe S, Bucksbaum P
Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
Department of Chemistry, Stanford University, Stanford, California 94305, USA.
Phys Rev Lett. 2015 Apr 10;114(14):143005. doi: 10.1103/PhysRevLett.114.143005.
Resonant Raman excitation by ultrafast vacuum ultraviolet laser pulses is a powerful means to study electron dynamics in molecules, but experiments must contend with linear background ionization: frequencies high enough to reach resonant core-valence transitions will usually ionize all occupied orbitals as well, and the ionization cross sections are usually dominant. Here we show that attosecond pulses can induce a process, transient impulsive stimulated Raman scattering, which can overwhelm valence ionization. Calculations are performed for atomic sodium, but the principal is valid for many molecular systems. This approach opens the path for high-fidelity multidimensional spectroscopy with attosecond pulses.
超快真空紫外激光脉冲产生的共振拉曼激发是研究分子中电子动力学的有力手段，但实验必须应对线性背景电离：频率高到足以达到共振芯价跃迁的同时通常也会使所有占据轨道电离，且电离截面通常占主导。本文我们表明阿秒脉冲能够诱导一个过程，即瞬态脉冲受激拉曼散射，它能够压制价电子电离。我们对钠原子进行了计算，但该原理对许多分子系统都有效。这种方法为利用阿秒脉冲进行高保真多维光谱学研究开辟了道路。
