Imaging an aligned polyatomic molecule with laser-induced electron diffraction

Laser-induced electron diffraction is an evolving tabletop method that aims to image ultrafast structural changes in gas-phase polyatomic molecules with sub-Ångström spatial and femtosecond temporal resolutions. Here we demonstrate the retrieval of multiple bond lengths from a polyatomic molecule by simultaneously measuring the C-C and C-H bond lengths in aligned acetylene. Our approach takes the method beyond the hitherto achieved imaging of simple diatomic molecules and is based on the combination of a 160 kHz mid-infrared few-cycle laser source with full three-dimensional electron-ion coincidence detection. Our technique provides an accessible and robust route towards imaging ultrafast processes in complex gas-phase molecules with atto- to femto-second temporal resolution.