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Contribution of multiple plasmon scattering in low-angle electron diffraction investigated by energy-filtered atomically resolved 4D-STEM

We report the influence of multiple plasmon losses on the dynamical diffraction of high-energy electrons, in a scanning transmission electron microscopy (STEM) study. Using an experimental setup enabling energy-filtered momentum-resolved STEM, it is shown that the successive excitation of up to five plasmons within the imaged material results in a subsequent and significant redistribution of low-angle intensity in diffraction space. An empirical approach, based on the convolution with a Lorentzian kernel, is shown to reliably model this redistribution in dependence of the energy-loss. Our study demonstrates that both the significant impact of inelastic scattering in low-angle diffraction at elevated specimen thickness and a rather straightforward model can be applied to mimic multiple plasmon scattering, which otherwise is currently not within reach for multislice simulations due to computational complexity.