Detecting charge transfer at defects in 2D materials with electron ptychography

Electronic charge transfer at the atomic scale can reveal fundamental information about chemical bonding, but is far more challenging to directly image than the atomic structure. The charge density is dominated by the atomic nuclei, with bonding causing only a small perturbation. Thus detecting any change due to bonding requires a higher level of sensitivity than imaging structure and the overall charge density. Here we achieve the sensitivity required to detect charge transfer in both pristine and defected monolayer WS\textsubscript{2} using the high dose efficiency of electron ptychography and its ability to correct for lens aberrations. Excellent agreement is achieved with first-principles image simulations including where thermal diffuse scattering is explicitly modeled via finite-temperature molecular dynamics based on density functional theory. The focused-probe ptychography configuration we use also provides the important ability to concurrently collect the annular dark-field signal, which can be unambiguously interpreted in terms of the atomic structure and chemical identity of the atoms, independently of the charge transfer. Our results demonstrate both the power of ptychographic reconstructions and the importance of quantitatively accurate simulations to aid their interpretation.