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Multiphoton ionization with three-dimensional light fields

D. Köhnke*, H.-C. Ahlswede*, T. Bayer, and M. Wollenhaupt†

  • *These authors contributed equally to this work.
  • †Contact author: matthias.wollenhaupt@uol.de

Phys. Rev. Research 8, 033048 – Published 13 July, 2026

DOI: https://doi.org/10.1103/r36b-vw82

Abstract

We employ, for the first time, bichromatic three-dimensional (3D) polarization-shaped ultrashort laser fields in atomic multiphoton ionization to create previously inaccessible free-electron angular momentum wave packets. The 3D fields are created by the noncollinear superposition of two polarization-shaped pulses of different colors from a supercontinuum polarization pulse shaper and provide electric-field components along all spatial directions. The resulting photoelectron momentum distributions, recorded via velocity map imaging, demonstrate full 3D quantum control of electronic superposition states extending beyond the constraints of planar polarization fields by unlocking all dipole selection rules Δm=0,±1. As an application, 3D pump-probe fields are used to map spin-orbit dynamics of the potassium 3d fine structure doublet. Our shaper-based approach establishes a route to fully controllable 3D light fields for chiral-sensitive light-matter interactions and ultrafast spectroscopy.

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