Coherent Raman beat electron paramagnetic resonance (EPR) spectra with
out application of one or more excitation pulses have been observed in
the EPR spectrum of the tetramethyl-1,4-benzosemiquinone anion radica
l in a frozen mixture (50:50) of protonated and fully deuterated isopr
opyl alcohol at 4.2 K. The free nuclear transition frequencies of hydr
ogen and deuterium and the small quadrupole coupling of 146 kHz of the
deuterium could be measured with high sensitivity and precision (line
width = approximate to 40 kHz). The modulation amplitudes of the deut
erium matrix lines at 2.2 MHz, as a function of the observer power, re
veal a distinct resonance behavior coinciding with the frequency of th
e transient nutations, that is, when the Rabi frequency is approximate
ly equal to the nuclear precession frequency. These observations sugge
st that the mechanism of coherence transfer between the electron and n
uclear spin systems is related to the Hartmann-Hahn effect.