Is there a Stobbs factor in atomic-resolution STEM-EELS mapping?

• This paper present a carefully calibrated experiment, which allows, for the first time, atomic-resolution chemical signals to be extracted on an absolute scale.
• By simultaneously recording the elastic signal, also on an absolute scale, all free parameters are eliminated in simulations of the core-loss signals.
• Coupled with double-channeling simulations, the present work enables a close scrutiny of the scattering physics in the inelastic channel.
• This paper demonstrates that element-specific atom counting within a single-particle picture is possible under favorable circumstances.

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.