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

Abstract

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 CD of up to 10% survives in the angularly-integrated above-threshold ionization (ATI) spectra, and of up to 5% in the total ionization rates. We demonstrate these results through ab-initio calculations in the chiral molecules Bromochlorofluoromethane, Limonene, Fenchone, and Camphor. We also explore the parameter-space of the locally-chiral field and show that the observed CD is strongly correlated to the degree of chirality of the light, validating it as a measure for chiral-interaction strengths. Our results pave the way for highly selective probing of ultrafast chirality in ATI, can potentially lead to all-optical enantio-separation, and motivate the use of locally-chiral light for enhancing ultrafast spectroscopies.

11 pages, 8 figures

References in corpus (8)

• 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
• A first principles TDDFT framework for spin and time-resolved ARPES in periodic systems
• Theoretical description of circular dichroism in photoelectron angular distributions of randomly oriented chiral molecules after multi-photon photoionization
• Efficient and accurate modeling of electron photoemission in nanostructures with TDDFT
• Strong Differential Photoion Circular Dichroism in Strong-Field Ionization of Chiral Molecules
• Photoelectron circular dichroism in the multiphoton ionization by short laser pulses: III. Photoionization of fenchone in different regimes

Cited by in corpus (8)

• Ultrafast chirality: the road to efficient chiral measurements
• The Application of Tailored Fields for Studying Chirality and Symmetry
• Detecting multiple chirality centers in chiral molecules with high harmonic generation
• Enantiosensitive steering of free-induction decay
• Unambiguous definition of handedness for locally-chiral light
• Phase-matched locally chiral light for global control of chiral light-matter interaction
• Chiral Electron Momentum Distribution upon Strong-Field Ionization of Atoms
• Multiphoton ionization with three-dimensional light fields