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.

arXiv comment8 pages, 6 figures, 1 page SM

References in corpus (16)

• Adam: A Method for Stochastic Optimization
• Relativistic separable dual-space Gaussian Pseudopotentials from H to Rn
• Topological response in Weyl semimetals and the chiral anomaly
• Real-space grids and the Octopus code as tools for the development of new simulation approaches for electronic systems
• Generation of phase-matched circularly-polarized extreme ultraviolet high harmonics for magnetic circular dichroism spectroscopy
• Octopus, a computational framework for exploring light-driven phenomena and quantum dynamics in extended and finite systems
• Weyl Semimetals, Fermi Arcs and Chiral Anomalies (A Short Review)
• Creating stable Floquet-Weyl semimetals by laser-driving of 3D Dirac materials
• Symmetries and selection rules in Floquet systems: application to harmonic generation in nonlinear optics
• Locally and globally chiral fields for ultimate control of chiral light matter interaction
• Weyl, Dirac and high-fold chiral fermions in topological quantum materials
• Enantiomer-Specific State Transfer of Chiral Molecules
• Highly selective chiral discrimination in high harmonic generation by dynamical symmetry breaking spectroscopy
• Real-time probing of chirality during a chemical reaction
• Probing molecular chirality via laser-induced electronic fluxes
• Strong chiral dichroism in above threshold ionization and ionization rates from locally-chiral light

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