Detecting multiple chirality centers in chiral molecules with high harmonic generation

Abstract

Characterizing chirality is highly important for applications in the pharmaceutical industry, as well as in the study of dynamical chemical and biological systems. However, this task has remained challenging, especially due to the ongoing increasing complexity and size of the molecular structure of drugs and active compounds. In particular, large molecules with many active chirality centers are today ubiquitous, but remain difficult to structurally analyze due to their high number of stereoisomers. Here we theoretically explore the sensitivity of high harmonic generation (HHG) to the chirality of molecules with a varying number of active chiral centers. We find that HHG driven by bi-chromatic non-collinear lasers is a sensitive probe for the stereo-configuration of a chiral molecule. We first show through calculations (from benchmark chiral molecules with up to three chirality centers) that the HHG spectrum is imprinted with information about the handedness of each chirality center in the driven molecule. Next, we show that using both classical- and deep-learning-based reconstruction algorithms, the composition of an unknown mixture of stereoisomers can be reconstructed with high fidelity by a single-shot HHG measurement. Our work illustrates how the combination of non-linear optics and machine learning might open routes for ultra-sensitive sensing in chiral systems.

8 pages, 6 figures, 1 page SM

References in corpus (3)

• Topological response in Weyl semimetals and the chiral anomaly
• Weyl Semimetals, Fermi Arcs and Chiral Anomalies (A Short Review)
• Enantiomer-Specific State Transfer of Chiral Molecules

Cited by in corpus (7)

• Ultrafast chirality: the road to efficient chiral measurements
• Are there universal signatures of topological phases in high harmonic generation? Probably not
• Molecular chirality and its monitoring by ultrafast X-ray pulses
• The Application of Tailored Fields for Studying Chirality and Symmetry
• Ab-initio cluster approach for high-harmonic generation in liquids
• Unambiguous definition of handedness for locally-chiral light
• Phase-matched locally chiral light for global control of chiral light-matter interaction