Imaging of isotope diffusion using atomic-scale vibrational spectroscopy

The spatial resolutions of even the most sensitive isotope analysis techniques based on light or ion probes are limited to a few hundred nanometres. Although vibrational spectroscopy using electron probes has achieved higher spatial resolution1-3, the detection of isotopes at the atomic level4 has been challenging so far. Here we show the unambiguous isotopic imaging of 12C carbon atoms embedded in 13C graphene and the monitoring of their self-diffusion via atomic-level vibrational spectroscopy. We first grow a domain of 12C carbon atoms in a pre-existing crack of 13C graphene, which is then annealed at 600 degrees Celsius for several hours. Using scanning transmission electron microscopy-electron energy loss spectroscopy, we obtain an isotope map that confirms the segregation of 12C atoms that diffused rapidly. The map also indicates that the graphene layer becomes isotopically homogeneous over 100-nanometre regions after 2 hours. Our results demonstrate the high mobility of carbon atoms during growth and annealing via self-diffusion. This imaging technique can provide a fundamental methodology for nanoisotope engineering and monitoring, which will aid in the creation of isotope labels and tracing at the nanoscale.