Abstract

An all-optical technique for distinguishing between chiral isomers of molecules yields much larger effects than current methods, paving the way for subfemtosecond resolution of chiral dynamics.

Highlights

  • The detection and characterization of chirality plays a central role in a broad range of sciences

  • The two schemes differ in the range of ellipticities at which the circular dichroism (CD) effect is studied and will be referred to as “bicircular” and “bielliptical.” Details on the optical implementation of these two schemes are given in the Appendix

  • The bicircular technique leads to relatively high levels of CD of up to 13% whereas the bielliptical technique leads to maximizing ellipticities of up to ∼4%

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Summary

Introduction

The detection and characterization of chirality plays a central role in a broad range of sciences. The development of ever more sensitive chiral spectroscopies has received considerable attention. Their basic principle relies on the interaction with light, which is itself chiral [e.g., circularly polarized light (CPL)] [1], as in optical rotatory dispersion [2], circular dichroism (CD), or Raman optical activity [3,4,5,6]. Several chiral-sensitive techniques have been developed for the gas phase. The sensitivity of these methods, such as three-wave-mixing microwave spectroscopy [9], Coulomb-explosion imaging [10,11,12,13], and laser-induced mass spectrometry [14,15], resides in the electric-dipole

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