Figure compares the EADS3 reported in Figure both with the absorption spectrum of the 1 n N * state and with the absorption spectrum of a linear combination of the 1 n N * and 1 n O * states. While the absorption spectrum of the 1 n N * state compares satisfactorily well with the EADS3, a 50%:50% linear combination of the absorption spectrum of the 1 n N * and either the planar or twisted 1 n O * states also seems to be in fair agreement. Note that the predicted absorption spectra of the planar and twisted 1 n O * minima are practically identical and, hence, do not affect the linear combination. We cannot rule out a minor participation of the 1 n O * state in the experimental data. However, we note that if both 1 n N * and 1 n O * excited states were populated in Cyd, their excited state decay lifetimes would be expected to be different from each other. Because the absorption spectrum of the 1 n O * state is predicted to have more intensity around 330 nm, while that of 1 n N * state is predicted to have more intensity around 420 nm and 550 nm (i.e., relative to each other), we have normalized the decay traces at these three probe wavelengths (see, Figure ). As can be seeing in Figure , the dynamics are practically identical within the signal-tonoise and decay in lock step with each other for kinetic traces at 330 nm and 420 nm, however the dynamics are vastly different at 550 nm. This provides strong experimental evidence that the EADS3 is primarily associated to a single transient species (the absorption of the 1 n N * state) and not to a combination of two or more transient species. This idea is further supported by quantum chemical calculations for cytosine and 1-methylcytosine that includes explicit water molecules, which have shown that the 1 n N * minimum is lower in energy than the 1 n O * minima, and the 1 n O * state is also significantly higher in energy in the Franck-Condon region, and should not be populated to any major extent upon excitation at 267 nm. For ease of comparison traces at 320 and 420 nm were normalized at ca. 5 ps, however due to the significantly smaller intensity of the signal at 550 nm this trace was plotted without normalization as to not highlight the noise of the data. Note the break around time zero, which is masking a strong coherent signal from the solvent at 330 nm.