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We performed STM-ENDOR experiments where the intensity of one of thehyperfine components detected in ESR-STM is recorded while an rf power isirradiated into the tunneling junction and its frequency is swept. When thelatter frequency is near a nuclear transition a dip in ESR-STM signal isobserved. This experiment was performed in three different systems: nearsurface SiC vacancies where the electron spin is coupled to a next nearestneighbor 29Si nucleus; Cu deposited on Si(111)7x7 surface, where the unpairedelectron of the Cu atom is coupled to the Cu nucleus (63Cu, 65Cu) and on Tempomolecules adsorbed on Au(111), where the unpaired electron is coupled toNitrogen nucleus (14N). While some of the hyperfine values are unresolved inthe ESR-STM data due to linewidth we find that they are accurately determinedin the STM-ENDOR data including those from remote nuclei, which are notdetected in the ESR-STM spectrum. Furthermore, STM-ENDOR can measure singlenuclear Zeeman frequencies, distinguish between isotopes through theirdifferent nuclear magnetic moments and detect quadrupole spectra. We alsodevelop and solve a Bloch type equation for the coupled electron-nuclear systemthat facilitates interpretation of the data. The improved spectral resolutionof STM - ENDOR opens many possibilities for nanometric scale chemical analysis.

Fingerprints of single nuclear spin energy levels using STM - ENDOR