Strong chiral dichroism in above threshold ionization and ionization rates from locally-chiral light.

  title={Strong chiral dichroism in above threshold ionization and ionization rates from locally-chiral light.},
  author={Ofer Neufeld and Hannes Hubener and {\'A}ngel Rubio and Umberto De Giovannini},
  journal={arXiv: Chemical Physics},
We derive here a new highly selective photoelectron-based chirality-sensing technique that utilizes 'locally-chiral' laser pulses. We show that this approach results in strong chiral discrimination, where the standard forwards/backwards asymmetry of photoelectron circular dichroism (PECD) is lifted. The resulting dichroism is much larger and more robust than conventional PECD, is found in all hemispheres, and is not symmetric or antisymmetric with respect to any symmetry operator. Remarkably, a… 

Figures and Tables from this paper



Photoexcitation circular dichroism in chiral molecules

Chiral effects appear in a wide variety of natural phenomena and are of fundamental importance in science, from particle physics to metamaterials. The standard technique of chiral

Chiral Discrimination through Bielliptical High-Harmonic Spectroscopy

Molecular chirality plays an essential role in most biochemical processes. The observation and quantification of chirality-sensitive signals, however, remains extremely challenging, especially on

General theory of photoexcitation induced photoelectron circular dichroism.

A general theory of PXECD is presented based on angular momentum algebra and explicit expressions for all pertinent asymmetry parameters which arise for the arbitrary polarization of pump (which prepares the superposition of excited states) and ionizing probe pulses are derived.

Universality of photoelectron circular dichroism in the photoionization of chiral molecules

Photoionization of chiral molecules by circularly polarized radiation gives rise to a strong forward/backward asymmetry in the photoelectron angular distribution, referred to as photoelectron

Attosecond-resolved photoionization of chiral molecules

Self-referenced attosecond photoelectron interferometry is implemented to measure the temporal profile of the forward and backward electron wave packets emitted upon photoionization of camphor by circularly polarized laser pulses, and reveals the chiral character of strongly correlated electronic dynamics.

Non-linear optical spectroscopy as a novel probe for molecular chirality

Optical second-harmonic generation and sum-frequency generation as novel spectroscopic tools to probe molecular chirality are currently being developed. The latter in particular allows studies of

Imaging photoelectron circular dichroism of chiral molecules by femtosecond multiphoton coincidence detection.

The electron-ion coincidence technique using multiphoton ionization opens new directions in table-top analytical mass-spectrometric applications of mixtures of chiral molecules.

Theoretical description of circular dichroism in photoelectron angular distributions of randomly oriented chiral molecules after multi-photon photoionization.

A theoretical framework describing this process as (2+1) resonantly enhanced multi-photon ionization is constructed and it is verified that the model correctly reproduces the basic symmetry behavior expected under exchange of handedness and light helicity.

Probing ultrafast dynamics of chiral molecules using time-resolved photoelectron circular dichroism.

It is shown that time-resolved PECD enables revealing dynamics much faster than the population decay of the Rydberg states, demonstrating the high sensitivity of this technique to vibronic relaxation.