Diffraction and microscopy with attosecond electron pulse trains

Attosecond spectroscopy1–7 can resolve electronic processes directly in time, but a movie-like space–time recording is impeded by the too long wavelength (~100 times larger than atomic distances) or the source–sample entanglement in re-collision techniques8–11. Here we advance attosecond metrology to picometre wavelength and sub-atomic resolution by using free-space electrons instead of higher-harmonic photons1–7 or re-colliding wavepackets8–11. A beam of 70-keV electrons at 4.5-pm de Broglie wavelength is modulated by the electric field of laser cycles into a sequence of electron pulses with sub-optical-cycle duration. Time-resolved diffraction from crystalline silicon reveals a < 10-as delay of Bragg emission and demonstrates the possibility of analytic attosecond–ångström diffraction. Real-space electron microscopy visualizes with sub-light-cycle resolution how an optical wave propagates in space and time. This unification of attosecond science with electron microscopy and diffraction enables space–time imaging of light-driven processes in the entire range of sample morphologies that electron microscopy can access.publishe