First, we test the accuracy and precision of the algorithm by model fitting to simulated data and comparing the fit parameters to known, true values. We simulate the isotropic response of the C≡N stretch of MeSCN in H2O as characterized by Yuan and Fayer. We add Gaussian noise (SNR ~600:1) to the free induction decay to simulate experimental data. Here we define signal in the SNR calculation as the peak magnitude of the 0-1 transition of the transient absorption spectrum at zero waiting time. Our choice to simulate data with 600:1 SNR avoids occasional unphysical results that would otherwise occur in the CLS analysis of data with lower SNR over the course of 100 trials. Nevertheless, we also show that model fitting can be reliable for data with SNR of 10:1 (vide infra) subject to the expected increase in variance predicted by Eq. 7.