The scanning transmission electron microscope (STEM) can capture a multitude of signals corresponding to the structural and chemical properties of a material. Examples of these methods include bright/dark field imaging, energy dispersive x-ray spectroscopy (EDS), or electron energy loss spectroscopy (EELS)[1]. EELS is of particular interest due to its sensitivity to low-mass elements and ability to determine their oxidation states, chemical bonding, and spatial distribution. An EEL spectrum is challenging to acquire due to low signals, energy spread of the beam, and the sensitivity of the detector. Furthermore, the stability of the sample is compromised due to the acquisition speed, which is a combination of signal limitations and camera read-out speed. One solution to overcome these limitations is the use of probe sub-sampling, whereby only a subset of probe locations is acquired with respect to the typical scanning …