▎ 摘　　要

Here, the authors perform lightwave-driven terahertz scanning tunnelling microscopy and spectroscopy of graphene nanoribbons with atomic resolution in three dimensions, revealing localized wavefunctions that are inaccessible by conventional scanning tunnelling microscopy. Atomically precise electronics operating at optical frequencies require tools that can characterize them on their intrinsic length and time scales to guide device design. Lightwave-driven scanning tunnelling microscopy is a promising technique towards this purpose. It achieves simultaneous sub-angstrom and sub-picosecond spatio-temporal resolution through ultrafast coherent control by single-cycle field transients that are coupled to the scanning probe tip from free space. Here, we utilize lightwave-driven terahertz scanning tunnelling microscopy and spectroscopy to investigate atomically precise seven-atom-wide armchair graphene nanoribbons on a gold surface at ultralow tip heights, unveiling highly localized wavefunctions that are inaccessible by conventional scanning tunnelling microscopy. Tomographic imaging of their electron densities reveals vertical decays that depend sensitively on wavefunction and lateral position. Lightwave-driven scanning tunnelling spectroscopy on the angstrom scale paves the way for ultrafast measurements of wavefunction dynamics in atomically precise nanostructures and future optoelectronic devices based on locally tailored electronic properties.