Ethylenedione C2O2 is one of the elusive small molecules which have remaine
d undetected even after numerous attempts with different experimental techn
iques, This is surprising, since theoretical studies predicted the triplet
state of C2O2 to be stable towards spin-allowed dissociation and hence long
-lived. Here we report a comprehensive study of charged and neutral ethylen
edione by means of charge reversal and neutralization -reionization mass sp
ectrometry. These experimental results, in conjunction with theoretical cal
culations, suggest that neutral ethylenedione is intrinsically short-lived
rather than being elusive, Both the singlet and triplet states of C2O2 are
predicted to dissociate rapidly into two ground-state CO molecules, and for
the triplet species, this dissociation involves facile curve-crossing to t
he singlet surface within a few nanoseconds.