Molecular quantum beats are observed in the isotropic fluorescence dec
ay following laser excitation of individual rotational states of C2N2
via the vibronically allowed 4(0)1 A(1SIGMA(U)-)<--X(1SIGMA(g)+) trans
ition near 219 nm. Strong quantum beats occur with selective excitatio
n, by both P- and R-branch transitions, of over a dozen rotational sta
tes. Observations of hyperfine quantum beats following excitation of t
he N' = 12 rotational level yield estimates of spin-orbit coupling mat
rix elements, Born-Oppenheimer state separations, and magnetic and qua
drupolar hyperfine coupling constants. Observations of Zeeman splittin
g establish that the three hyperfine levels of N' = 12 are coupled to
those of a single triplet state.