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Scanning probe microscopy (SPM) has revolutionized the fields of materials, nano-science, chemistry, and biology, by enabling mapping of surface properties and surface manipulation with atomic precision. However, these achievements require constant human supervision; fully automated SPM has not been accomplished yet. Here we demonstrate an artificial intelligence framework based on machine learning for autonomous SPM operation (DeepSPM). DeepSPM, an autonomous artificial intelligence (AI)-driven scanning probe microscope | A. Krull, P. Hirsch, C. Rother, A. Schiffrin & C. Krull