Photoelectron circular dichroism observed in the above-threshold ionization signal from chiral molecules with femtosecond laser pulses

Abstract

Photoelectron circular dichroism is investigated experimentally as a function of the number of absorbed circularly polarized photons. Three structurally different chiral molecules yet showing similar absorption spectra are studied. They are isotropically distributed in the gas phase and ionized with femtosecond laser pulses. We measure and analyze the photoelectron angular distribution of threshold electrons ionized with three photons and compare them to those of above-threshold (ATI) electrons ionized with four photons. Additionally to an increase in high even order Legendre polynomials the coefficients of the high odd order Legendre polynomials rise with increasing photon number. Consequently, the ATI electrons also carry the chirality signature. All investigated chiral molecules reveal an individual set of coefficients for the threshold and ATI signatures despite their similarities in chemical structure. The presented data set can serve as a guideline for theoretical modeling of the interaction of circularly polarized light with chiral molecules in the multiphoton regime.