J. R. Macdonald Laboratory, Physics Department, Kansas State University, Manhattan, Kansas 66506-2604, USA.
Phys Chem Chem Phys. 2012 Oct 14;14(38):13133-45. doi: 10.1039/c2cp41606a.
We introduce a laser-induced electron diffraction method (LIED) for imaging ultrafast dynamics of small molecules with femtosecond mid-infrared lasers. When molecules are placed in an intense laser field, both low- and high-energy photoelectrons are generated. According to quantitative rescattering (QRS) theory, high-energy electrons are produced by a rescattering process where electrons born at the early phase of the laser pulse are driven back to rescatter with the parent ion. From the high-energy electron momentum spectra, field-free elastic electron-ion scattering differential cross sections (DCS), or diffraction images, can be extracted. With mid-infrared lasers as the driving pulses, it is further shown that the DCS can be used to extract atomic positions in a molecule with sub-angstrom spatial resolution, in close analogy to the standard electron diffraction method. Since infrared lasers with pulse duration of a few to several tens of femtoseconds are already available, LIED can be used for imaging dynamics of molecules with sub-angstrom spatial and a few-femtosecond temporal resolution. The first experiment with LIED has shown that the bond length of oxygen molecules shortens by 0.1 Å in five femtoseconds after single ionization. The principle behind LIED and its future outlook as a tool for dynamic imaging of molecules are presented.
我们介绍了一种激光诱导电子衍射方法(LIED),用于使用飞秒中红外激光对小分子的超快动力学进行成像。当分子置于强激光场中时,会同时产生低能和高能光电子。根据定量再散射(QRS)理论,高能电子是通过再散射过程产生的,其中在激光脉冲早期产生的电子被驱回与母离子再散射。从高能电子动量谱中,可以提取无场弹性电子-离子散射微分截面(DCS)或衍射图像。使用中红外激光作为驱动脉冲,进一步表明 DCS 可用于以亚埃空间分辨率提取分子中的原子位置,与标准电子衍射方法非常相似。由于已经有几到几十飞秒的几到几十飞秒的红外激光可用,LIED 可用于以亚埃空间和几飞秒时间分辨率成像分子动力学。LIED 的第一个实验表明,单电离后五个飞秒内氧分子的键长缩短了 0.1Å。本文介绍了 LIED 的原理及其作为分子动态成像工具的未来前景。