Photoelectron Circular Dichroism in the Spin-Polarized Spectra of Chiral Molecules.

We studied strong-field multiphoton ionization of 1-iodo-2-methylbutane enantiomers with 395 nm circularly polarized laser pulses experimentally and theoretically. For randomly oriented molecules, we observe spin polarization up to about 15%, which is independent of the molecular enantiomer. Our experimental findings are explained theoretically as an intricate interplay between three contributions from HOMO, HOMO-1, and HOMO-2, which are formed of 5p-electrons of the iodine atom. For uniaxially oriented molecules, our theory demonstrates even larger spin polarization. Moreover, we predict a sizable enantiosensitive photoelectron circular dichroism of about 10%, which is different for different spin states of photoelectrons.