JILA, Department of Physics, University of Colorado and National Institute of Standards and Technology, Boulder, CO 80309.
JILA, Department of Physics, University of Colorado and National Institute of Standards and Technology, Boulder, CO 80309;
Proc Natl Acad Sci U S A. 2017 Jul 3;114(27):E5300-E5307. doi: 10.1073/pnas.1706466114. Epub 2017 Jun 19.
Electron-electron interactions are the fastest processes in materials, occurring on femtosecond to attosecond timescales, depending on the electronic band structure of the material and the excitation energy. Such interactions can play a dominant role in light-induced processes such as nano-enhanced plasmonics and catalysis, light harvesting, or phase transitions. However, to date it has not been possible to experimentally distinguish fundamental electron interactions such as scattering and screening. Here, we use sequences of attosecond pulses to directly measure electron-electron interactions in different bands of different materials with both simple and complex Fermi surfaces. By extracting the time delays associated with photoemission we show that the lifetime of photoelectrons from the band of Cu are longer by ∼100 as compared with those from the same band of Ni. We attribute this to the enhanced electron-electron scattering in the unfilled band of Ni. Using theoretical modeling, we can extract the contributions of electron-electron scattering and screening in different bands of different materials with both simple and complex Fermi surfaces. Our results also show that screening influences high-energy photoelectrons (≈20 eV) significantly less than low-energy photoelectrons. As a result, high-energy photoelectrons can serve as a direct probe of spin-dependent electron-electron scattering by neglecting screening. This can then be applied to quantifying the contribution of electron interactions and screening to low-energy excitations near the Fermi level. The information derived here provides valuable and unique information for a host of quantum materials.
电子-电子相互作用是材料中最快的过程,其发生时间尺度在飞秒到阿秒之间,具体取决于材料的电子能带结构和激发能量。这种相互作用在光诱导过程中起着主导作用,例如纳米增强等离激元和催化、光捕获或相变。然而,迄今为止,还不可能从实验上区分散射和屏蔽等基本电子相互作用。在这里,我们使用阿秒脉冲序列直接测量不同材料不同能带中的电子-电子相互作用,这些材料具有简单和复杂的费米面。通过提取与光电子发射相关的时间延迟,我们表明,与 Ni 相同能带中的光电子相比,Cu 能带中的光电子的寿命长约 100。我们将这归因于 Ni 未填充的能带中增强的电子-电子散射。使用理论建模,我们可以从具有简单和复杂费米面的不同材料的不同能带中提取电子-电子散射和屏蔽的贡献。我们的结果还表明,屏蔽对高能光电子(≈20 eV)的影响远小于低能光电子。因此,通过忽略屏蔽,可以将高能光电子用作自旋相关电子-电子散射的直接探针。然后可以将其应用于量化费米能级附近低能激发的电子相互作用和屏蔽的贡献。这里得出的信息为一系列量子材料提供了有价值且独特的信息。