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Transmission electron microscopy and spectroscopy currently enable theacquisition of spatially resolved spectral information from a specimen byfocusing electron beams down to a sub-Angstrom spot and then analyzing theenergy of the inelastically scattered electrons with few-meV energy resolution.This technique has recently been used to experimentally resolve vibrationalmodes in 2D materials emerging at mid-infrared frequencies. Here, based onfirst-principles theory, we demonstrate the possibility of identifying singleisotope atom impurities in a nanostructure through the trace that they leave inthe spectral and spatial characteristics of the vibrational modes.Specifically, we examine a hexagonal boron nitride molecule as an example ofapplication, in which the presence of a single isotope impurity is revealedthrough dramatic changes in the electron spectra, as well as in the space-,energy-, and momentum-resolved inelastic electron signal. We compare theseresults with conventional far-field spectroscopy, showing that electron beamsoffer superior spatial resolution combined with the ability to probe thecomplete set of vibrational modes, including those that are optically dark. Ourstudy is relevant for the atomic-scale characterization of vibrational modes innovel materials, including a detailed mapping of isotope distributions.

Atomic-Scale Vibrational Mapping and Isotope Identification with Electron Beams