Xin Huolin L, Dwyer Christian, Muller David A
Department of Physics, Cornell University, Ithaca, NY 14853, USA.
Monash Centre for Electron Microscopy, ARC Centre of Excellence for Design in Light Metals, Monash University, Clayton, 3800 Vic, Australia; Department of Materials Engineering, Monash University, Clayton, 3800 Vic, Australia.
Ultramicroscopy. 2014 Apr;139:38-46. doi: 10.1016/j.ultramic.2014.01.006. Epub 2014 Jan 25.
Recent work has convincingly argued that the Stobbs factor-disagreement in contrast between simulated and experimental atomic-resolution images-in ADF-STEM imaging can be accounted for by including the incoherent source size in simulation. However, less progress has been made for atomic-resolution STEM-EELS mapping. Here we have performed carefully calibrated EELS mapping experiments of a [101] DyScO3 single-crystal specimen, allowing atomic-resolution EELS signals to be extracted on an absolute scale for a large range of thicknesses. By simultaneously recording the elastic signal, also on an absolute scale, and using it to characterize the source size, sample thickness and inelastic mean free path, we eliminate all free parameters in the simulation of the core-loss signals. Coupled with double channeling simulations that incorporate both core-loss inelastic scattering and dynamical elastic and thermal diffuse scattering, the present work enables a close scrutiny of the scattering physics in the inelastic channel. We found that by taking into account the effective source distribution determined from the ADF images, both the absolute signal and the contrast in atomic-resolution Dy-M5 maps can be closely reproduced by the double-channeling simulations. At lower energy losses, discrepancies are present in the Sc-L2,3 and Dy-N4,5 maps due to the energy-dependent spatial distribution of the background spectrum, core-hole effects, and omitted complexities in the final states. This work has demonstrated the possibility of using quantitative STEM-EELS for element-specific column-by-column atom counting at higher energy losses and for atomic-like final states, and has elucidated several possible improvements for future theoretical work.
近期的研究令人信服地表明,在环形暗场扫描透射电子显微镜(ADF-STEM)成像中,斯托布斯因子(即模拟与实验原子分辨率图像之间的对比度差异)可以通过在模拟中纳入非相干源尺寸来解释。然而,在原子分辨率的扫描透射电子显微镜-电子能量损失谱(STEM-EELS)mapping方面进展较小。在此,我们对[101]DyScO3单晶样品进行了精心校准的EELS mapping实验,从而能够在大范围厚度上以绝对尺度提取原子分辨率的EELS信号。通过同时也以绝对尺度记录弹性信号,并利用它来表征源尺寸、样品厚度和非弹性平均自由程,我们消除了模拟核心损失信号中的所有自由参数。结合包含核心损失非弹性散射以及动态弹性和热漫散射的双通道模拟,本工作能够对非弹性通道中的散射物理进行仔细研究。我们发现,通过考虑从ADF图像确定的有效源分布,双通道模拟能够紧密再现原子分辨率Dy-M5图中的绝对信号和对比度。在较低能量损失下,由于背景谱的能量相关空间分布、芯孔效应以及末态中被忽略的复杂性,Sc-L2,3和Dy-N4,5图中存在差异。这项工作证明了在较高能量损失下使用定量STEM-EELS进行逐列元素特异性原子计数以及针对类原子末态的可能性,并阐明了未来理论工作的一些可能改进方向。