Submolecular imaging by atomic force microscopy (AFM) has recently been established as a stunning technique to reveal the chemical structure of unknown molecules, to characterize intramolecular charge distributions and bond ordering, as well as to study chemical transformations and intermolecular interactions. So far, most of these feats were achieved on planar molecular systems because high-resolution imaging of three-dimensional (3D) surface structures with AFM remains challenging. Here we present a method for high-resolution imaging of nonplanar molecules and 3D surface systems using AFM with silicon cantilevers as force sensors. We demonstrate this method by resolving the step-edges of the (101) anatase surface at the atomic scale by simultaneously visualizing the structure of a pentacene molecule together with the atomic positions of the substrate and by resolving the contour and probe-surface force field on a C60 molecule with intramolecular resolution. The method reported here holds substantial promise for the study of 3D surface systems such as nanotubes, clusters, nanoparticles, polymers, and biomolecules using AFM with high resolution.

§Institute of Physics Academy of Sciences of the Czech Republic Cukrovarnicka 10 Prague Czech Rebublic

§JST PRESTO 4 1 8 Honcho Kawaguchi Saitama 332 0012 Japan

†National Institute for Materials Science 1 2 1 Sengen 305 0047 Tsukuba Ibaraki Japan

‡International Center for Young Scientists NIMS 1 2 1 Sengen 305 0047 Tsukuba Ibaraki Japan

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