Robust inversion of time-resolved data via forward-optimisation in a trajectory basis

TL;DR

This paper introduces a robust inversion method for time-resolved ultrafast experimental data using forward-optimisation in a trajectory basis, effectively handling noise and continuity constraints, and successfully applied to x-ray scattering and electron diffraction data.

Contribution

The paper presents a novel inversion approach that explicitly incorporates continuity constraints and demonstrates robustness against noise in ultrafast data analysis.

Findings

Successfully applied to x-ray scattering data of ring-opening reaction

Accurately models electron diffraction of CS2 dissociation

Reproduces experimental data and aligns with independent observations

Abstract

An inversion method for time-resolved data from ultrafast experiments is introduced, based on forward-optimisation in a trajectory basis. The method is applied to experimental data from x-ray scattering of the photochemical ring-opening reaction of 1,3-cyclohexadiene and electron diffraction of the photodissociation of CS2. In each case, inversion yields a model that reproduces the experimental data, identifies the main dynamic motifs, and agrees with independent experimental observations. Notably, the method explicitly accounts for continuity constraints and is robust for noisy data.