Diffraction using laser-driven broadband electron wave packets

Directly monitoring atomic motion during a molecular transformation with atomic-scale spatio-temporal resolution is a frontier of ultrafast optical science and physical chemistry. Here we provide the foundation for a new imaging method, fixed-angle broadband laser-induced electron scattering, based on structural retrieval by direct one-dimensional Fourier transform of a photoelectron energy distribution observed along the polarization direction of an intense ultrafast light pulse. The approach exploits the scattering of a broadband wave packet created by strong-field tunnel ionization to self-interrogate the molecular structure with picometer spatial resolution and bond specificity. With its inherent femtosecond resolution, combining our technique with molecular alignment can, in principle, provide the basis for time-resolved tomography for multi-dimensional transient structural determination.