Data for publication "Elucidating the Control of Circular Dichroism in Ion Yield via Chirped Pulses with Tailored Models"

We theoretically investigate circular dichroism in the ion yield following 1 + 1 + 1 ionization of3-methylcyclopentanone using femtosecond linearly chirped laser pulses, inspired by recent experi-ments by Das et al. [Phys. Chem. Chem. Phys. 27, 8043 (2025)]. To this end, we numerically solvethe time-dependent Schrödinger equation and evaluate the total population in the Rydberg statesat the end of the second absorption step. The A-band transition in the first absorption step istreated using state-of-the-art quantum-chemical calculations, whereas the second absorption step isdescribed via an effective model. Within our framework, we identify the interplay between the firstand second absorption step as the key explanation for the experimentally observed chirp depen-dence of the anisotropy. By elucidating this mechanism for the chirp-enhanced signal, our findingscontribute towards the development of improved control schemes for chiral molecules.