TY - JOUR
T1 - Is there a Stobbs factor in atomic-resolution STEM-EELS mapping?
AU - Xin, Huolin L.
AU - Dwyer, Christian
AU - Muller, David A.
N1 - Funding Information:
Funded by the Energy Materials Center at Cornell, an Energy Frontier Research Center (DOE #DE-SC0001086 ). This work made use of the Cornell Center for Materials Research Shared Facilities which are supported through the NSF MRSEC program ( DMR-1120296 ). C.D. would like to thank Philip Chan, eSolutions-Research Support Services and the Monash e-Research Centre for the use of Monash Central HPC cluster, and acknowledges financial support from the Australian Research Council ( DP110104734 ). Author contributions: H.L.X. conceived, designed, and performed the quantitative experiments, carried out the elastic scattering simulations and analyzed the experimental data. C.D. wrote the code for and performed the inelastic scattering simulations. C.D. and H.L.X. wrote the manuscript. All authors contributed to the discussions and know the implications of the results. Correspondence and requests for materials should be addressed to H.L.X.
PY - 2014/4
Y1 - 2014/4
N2 - 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.
AB - 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.
KW - Atomic resolution STEM-EELS
KW - Delocalization
KW - Double channeling
KW - Inelastic scattering
KW - Stobbs factor
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U2 - 10.1016/j.ultramic.2014.01.006
DO - 10.1016/j.ultramic.2014.01.006
M3 - Article
C2 - 24561427
AN - SCOPUS:84894103140
SN - 0304-3991
VL - 139
SP - 38
EP - 46
JO - Ultramicroscopy
JF - Ultramicroscopy
ER -