The following 4D-STEM data sets were collected on the ThemIS and TitanX scanning transmission electron microscopes located at the National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, USA. 1• Au_thermal_beforeHT_17C.dm4, Au_thermal_HT_800C.dm4, Au_thermal_HT_1000C.dm4 and Au_thermal_afterHT_17C.dm4 are datasets from 4D-STEM measurements conducted in situ on an FEI ThemIS image corrected microscope at 300 kV during a thermal cycling experiment. These digital micrograph (.dm4) files were collected at 17 C before heat treatment, 800 C during heat treatment, 1000 C during heat treatment, and 17 C after heat treatment, respectively. Nano-diffraction data was collected using a Gatan K2-IS (2k x 2k) detector at 400 frames per second. Each dataset contains a set of electron diffraction patterns taken at each scan position with a ~ 1 nm probe step size. Approximately 80 x 80 scan positions were recorded from each region with a dwell time of 0.0025 seconds per frame. A custom 40µm patterned “bullseye” circular probe forming aperture was used to enhance the accuracy of 4D-STEM strain analysis by facilitating the identification of the center of diffraction discs. A convergence angle of 3.20 milli-radians, spot size of 8, and diffraction pixel size of 0.16 Å-1 was used in micro-probe lens configuration. The data was machine and software binned to 512 x 512 pixels to increase the signal to noise ratio before computational analysis. Data processing were performed using strain mapping scripts provided in the open source py4DSTEM software package. Au_thermal_calibration.h5 contains the py4DSTEM calibration and diffraction standard data from the analysis. Polycrystalline Al standard sample was used to calibrate the reciprocal space pixel size as well as measure the elliptical distortion present in the data set. 2• Al_irradiated.dm4 is a dataset from 4D-STEM measurement conducted in situ on an FEI TitanX microscope equipped to do high-angle STEM tomography and operating at 300 kV. Nano-diffraction data was acquired using a Gatan Orius 830 (2k x 2k) detector capable of collecting 30 frames per second. Each dataset contains a stack of convergent beam electron diffraction (CBED) patterns taken at each scan position with maximum resolution equivalent to 1.6 nm probe size. Approximately 50 x 50 frame scan regions were recorded with a dwell time of 0.01 seconds per frame. A custom 70 µm patterned “bullseye” circular C2 aperture was used to greatly enhance the accuracy of 4D-STEM strain analysis by facilitating the identification of the center of diffraction discs. A convergence angle of 2.7 milli-radians, spot size 10, and camera length 195 mm was used in micro-probe lens configuration. With a measured screen current of 300 pA in this configuration, the total sum of electrons incident in a region of the sample, commonly known as the fluence (total dose), was determined at 67,100 electronsÅ-2 per 4D-STEM scan. The 4D-STEM data was machine and software binned to 512 x 512 pixels to increase the signal to noise ratio before computational analysis. Al_irradiated_calibration.h5 contains the py4DSTEM calibration and diffraction standard data from the analysis. Polycrystalline Al standard sample was used to calibrate the reciprocal space pixel size as well as measure the elliptical distortion present in the data set.