Nanoscale diffractive probing of strain dynamics in ultrafast transmission electron microscopy

The control of optically driven high-frequency strain waves in nanostructured systems is an essential ingredient for the further development of nanophononics. However, broadly applicable experimental means to quantitatively map such structural distortion on their intrinsic ultrafast time and nanometer length scales are still lacking. Here, we introduce ultrafast convergent beam electron diffraction (U-CBED) with a nanoscale probe beam for the quantitative retrieval of the time-dependent local distortion tensor. We demonstrate its capabilities by investigating the ultrafast acoustic deformations close to the edge of a single-crystalline graphite membrane. Tracking the structural distortion with a 28-nm/700-fs spatio-temporal resolution, we observe an acoustic membrane breathing mode with spatially modulated amplitude, governed by the optical near field structure at the membrane edge. Furthermore, an in-plane polarized acoustic shock wave is launched at the membrane edge, which triggers secondary acoustic shear waves with a pronounced spatio-temporal dependency. The experimental findings are compared to numerical acoustic wave simulations in the continuous medium limit, highlighting the importance of microscopic dissipation mechanisms and ballistic transport channels

Nanoscale mapping of ultrafast magnetization dynamics with femtosecond Lorentz microscopy

Novel time-resolved imaging techniques for the investigation of ultrafast nanoscale magnetization dynamics are indispensable for further developments in light-controlled magnetism. Here, we introduce femtosecond Lorentz microscopy, achieving a spatial resolution below 100 nm and a temporal resolution of 700 fs, which gives access to the transiently excited state of the spin system on femtosecond timescales and its subsequent relaxation dynamics. We demonstrate the capabilities of this technique by spatio-temporally mapping the light-induced demagnetization of a single magnetic vortex structure and quantitatively extracting the evolution of the magnetization field after optical excitation. Tunable electron imaging conditions allow for an optimization of spatial resolution or field sensitivity, enabling future investigations of ultrafast internal dynamics of magnetic topological defects on 10-nanometer length scales

High-purity free-electron momentum states prepared by three-dimensional optical phase modulation

We demonstrate the quantized transfer of photon energy and transverse momentum to a high-coherence electron beam. In an ultrafast transmission electron microscope, a three-dimensional phase modulation of the electron wavefunction is induced by transmitting the beam through a laser-illuminated thin graphite sheet. This all-optical free-electron phase space control results in high-purity superpositions of linear momentum states, providing an elementary component for optically programmable electron phase plates and beam splitters

Coulomb-correlated electron number states in a transmission electron microscope beam

We demonstrate the generation of Coulomb-correlated pair, triple and quadruple states of free electrons by femtosecond photoemission from a nanoscale field emitter inside a transmission electron microscope. Event-based electron spectroscopy allows a spatial and spectral characterization of the electron ensemble emitted by each laser pulse. We identify distinctive energy and momentum correlations arising from acceleration-enhanced interparticle energy exchange, revealing strong few-body Coulomb interactions at an energy scale of about two electronvolts. State-sorted beam caustics show a discrete increase in virtual source size and longitudinal source shift for few-electron states, associated with transverse momentum correlations. We observe field-controllable electron antibunching, attributed primarily to transverse Coulomb deflection. The pronounced spatial and spectral characteristics of these electron number states allow filtering schemes that control the statistical distribution of the pulse charge. In this way, the fraction of specific few-electron states can be actively suppressed or enhanced, facilitating the preparation of highly non-Poissonian electron beams for microscopy and lithography, including future heralding schemes and correlated multi-electron probing

Probing chirality with inelastic electron-light scattering

Circular dichroism spectroscopy is an essential technique for understanding molecular structure and magnetic materials, but spatial resolution is limited by the wavelength of light, and sensitivity sufficient for single-molecule spectroscopy is challenging. We demonstrate that electrons can efficiently measure the interaction between circularly polarized light and chiral materials with deeply sub-wavelength resolution. By scanning a nanometer-sized focused electron beam across an optically-excited chiral nanostructure and measuring the electron energy spectrum at each probe position, we produce a high-spatial-resolution map of near-field dichroism. This technique offers a nanoscale view of a fundamental symmetry and could be employed as "photon staining" to increase biomolecular material contrast in electron microscopy