Highly selective chiral discrimination in high harmonic generation by dynamical symmetry breaking spectroscopy
arXiv:1807.02630 · doi:10.1103/PhysRevX.9.031002
Abstract
We propose and numerically demonstrate a new very robust and highly selective method for femtosecond time-resolved chiral spectroscopy using high harmonic generation (HHG). The method is based on dynamical symmetry breaking from chiral media, and relies only on intense electric-dipole transitions, and not on the interplay of electric and magnetic dipoles. The symmetry breaking results in the emission of a strong chiral signal in the form of otherwise 'forbidden' harmonics (i.e., that are not emitted from achiral media). The intensity of these symmetry-forbidden harmonics is directly correlated to the media's enantiomeric excess, yielding chiral selectivity. On the contrary, the strength of the 'allowed' harmonics is chiral-independent, hence they can be used as a reference to provide chiral selectivity from a single measurement, unlike previous time-resolved schemes that require multiple measurements. We demonstrate numerically 96% discrimination level from microscopic gas phase emission, outperforming by far previous time-resolved methods (the selectivity should be further enhanced when the HHG process is phase matched). We expect the new method to give rise to precise table-top characterization of chiral media in the gas-phase, and for highly sensitive time-resolved ultrafast probing of dynamical chiral processes.
References in corpus (13)
- Optimization Algorithm for the Generation of ONCV Pseudopotentials
- 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
- Symmetries and selection rules in Floquet systems: application to harmonic generation in nonlinear optics
- Attosecond-resolved photoionization of chiral molecules
- Enantiomer-Specific State Transfer of Chiral Molecules
- Relaxation Dynamics in Photoexcited Chiral Molecules Studied by Time-Resolved Photoelectron Circular Dichroism: Toward Chiral Femtochemistry
- Generalized perspective on chiral measurements without magnetic interactions
- Optical chirality in high harmonic generation
- Opportunities for chiral discrimination using high harmonic generation in tailored laser fields
- Theoretical description of circular dichroism in photoelectron angular distributions of randomly oriented chiral molecules after multi-photon photoionization
- Strong-field control and enhancement of chiral response in bi-elliptical high-order harmonic generation: an analytical model
- General theory of photoexcitation induced photoelectron circular dichroism
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