Strong confinement of charges in few-electron systems such as in atoms, molecules, and quantum dots leads to a spectrum of discrete energy levels often shared by several degenerate states. Because the electronic structure is key to understanding their chemical properties, methods that probe these energy levels in situ are important. We show how electrostatic force detection using atomic force microscopy reveals the electronic structure of individual and coupled self-assembled quantum dots. An electron addition spectrum results from a change in cantilever resonance frequency and dissipation when an electron tunnels on/off a dot. The spectra show clear level degeneracies in isolated quantum dots, supported by the quantitative measurement of predicted temperature-dependent shifts of Coulomb blockade peaks. Scanning the surface shows that several quantum dots may reside on what topographically appears to be just one. Relative coupling strengths can be estimated from these images of grouped coupled dots.nanoelectronics | single-electron charging | shell structure | electrostatic force microscopy T he ability to confine single charges at discrete energy levels makes semiconductor quantum dots (QDs) promising candidates as a platform for quantum computation (1, 2) and singlephoton sources (3). Tremendous progress has been made not only in understanding the properties of single electrons in QDs but also in controlling their quantum states, which is an essential prerequisite for quantum computation (4). Single-electron transport measurements have been the main experimental technique for investigating electron tunneling into QDs (5). Charge sensing techniques using built-in charge sensors, such as quantum point contacts (6), complement transport measurements because lower electron tunneling rates can be monitored with even real-time detection being possible (7). It is instrumentally challenging to study self-assembled QDs via conventional transport and charge sensing methods because of the difficulty in attaching electrodes. Although progress is being made (8-12), these techniques have very small yield and therefore make it difficult to assess variation in QD electronic properties. Compared to typical QDs studied via transport measurements, in particular lithographically defined QDs, self-assembled QDs can be fabricated to have smaller sizes, stronger confinement potentials, and a more scalable fabrication process, all of which make them attractive for practical applications.In this paper, we focus on an alternative technique for studying QDs that is better suited for self-assembled QDs: charge sensing by atomic force microscopy (AFM). Charge sensing by AFM is a convenient method to study the electronic structure of QDs because nanoelectrodes are not required and large numbers of QDs can be investigated in one experiment. Termed single-electron electrostatic force microscopy (e-EFM), this technique relies on the high force sensitivity of AFM to detect the electrostatic force resulting from single electrons tunneling into ...