Elucidating the Control of Circular Dichroism in Ion Yield via Chirped Pulses with Purposeful Models
We theoretically investigate circular dichroism in the ion yield following $1+1+1$ ionization of 3-methylcyclopentanone using femtosecond linearly chirped laser pulses, inspired by recent experiments by Das et al. [Phys. Chem. Chem. Phys. 27, 8043 (2025)]. To this end, we numerically solve the time-dependent Schrödinger equation and evaluate the total population in the Rydberg states at the end of the second absorption step. The A-band transition in the first absorption step is treated using state-of-the-art quantum-chemical calculations, whereas the second absorption step is described via an effective model. Within our framework, we identify the interplay between the first and second absorption step as the key explanation for the experimentally observed chirp dependence of the anisotropy. By elucidating this mechanism for the chirp-enhanced signal, our findings contribute towards the development of improved control schemes for chiral molecules.