Abstract
A new experimental technique, pulsed electron-nuclear-electron triple resonance spectroscopy, is demonstrated. It is based on a modification of the pulse sequence for electron-nuclear double resonance (ENDOR) in which two EPR and one NMR transition are irradiated. The irradiation of one EPR transition is detected via a second EPR transition. The nuclear hyperfine coupling, which separates these EPR transition frequencies, is the irradiated NMR transition. The major advantages of triple resonance spectroscopy include the ability to resolve overlapping nuclear resonances in the ENDOR spectrum and a more direct quantitative assignment of nuclear hyperfine and quadrupole couplings. The triple resonance experiment is an alternative to the recently proposed method of employing rapid magnetic field jumps between microwave pulses for generating hyperfine selective ENDOR spectra.
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