The spatial resolution of a scanning tunneling microscope (STM) can be enhanced using light element-terminated probes with spatially localized electron orbitals at the apex atom. Conductive diamond probes can provide carbon atomic orbitals suitable for STM imaging with sub-Ångström lateral resolution and high apex stability crucial for the small tunneling gaps necessary for high-resolution experiments. Here we demonstrate that high spatial resolution can be achieved in STM experiments with single-crystal diamond tips, which are generally only considered for use as probes for atomic force microscopy. The results of STM experiments with a heavily boron-doped, diamond probe on a graphite surface; density functional theory calculations of the tip and surface electronic structure; and first-principles tunneling current calculations demonstrate that the highest spatial resolution can be achieved with diamond tips at tip–sample distances of 3–5 Å when frontier p-orbitals of the tip provide their maximum contribution to the tunneling current. At the same time, atomic resolution is feasible even at extremely small gaps with very high noise in the tunneling current.
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