Tailored high-contrast attosecond electron pulses for coherent excitation and scattering

Temporally shaping the density of electron beams using light forms the basis for a wide range of established and emerging technologies, including free-electron lasers and attosecond electron microscopy. The modulation depth of compressed electron pulses is a key figure of merit limiting applications. In this work, we present an approach for generating background-free attosecond electron pulse trains by sequential inelastic electron-light scattering. Harnessing quantum interference in the fractional Talbot effect, we suppress unwanted background density in electron compression by several orders of magnitude. Our results will greatly enhance applications of coherent electron-light scattering, such as stimulated cathodoluminescence and streaking

Attosecond electron pulse trains and quantum state reconstruction in ultrafast transmission electron microscopy

Ultrafast electron and X-ray imaging and spectroscopy are the basis for an ongoing revolution in the understanding of dynamical atomic-scale processes in matter. The underlying technology relies heavily on laser science for the generation and characterization of ever shorter pulses. Recent findings suggest that ultrafast electron microscopy with attosecond-structured wavefunctions may be feasible. However, such future technologies call for means to both prepare and fully analyse the corresponding free-electron quantum states. Here, we introduce a framework for the preparation, coherent manipulation and characterization of free-electron quantum states, experimentally demonstrating attosecond electron pulse trains. Phase-locked optical fields coherently control the electron wavefunction along the beam direction. We establish a new variant of quantum state tomography—‘SQUIRRELS’—for free-electron ensembles. The ability to tailor and quantitatively map electron quantum states will promote the nanoscale study of electron–matter entanglement and new forms of ultrafast electron microscopy down to the attosecond regime

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

We observe Coulomb-correlated electron pair and triple states generated by femtosecond photoemission from a nanoscale field emitter inside a transmission electron microscope. Event-based electron spectroscopy allows for spatial and spectral characterization of the electrons emitted by each laser pulse. Distinctive energy and momentum correlations of two- and three-electron states are identified, revealing a strong few-body Coulomb interaction 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. The pronounced spatial and spectral characteristics of these electron number states allow for 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 schemes in correlated two-electron probing

Light-induced hexatic state in a layered quantum material

The tunability of materials properties by light promises a wealth of future applications in energy conversion and information technology. Strongly correlated materials such as transition-metal dichalcogenides (TMDCs) offer optical control of electronic phases, charge ordering and interlayer correlations by photodoping. Here, we find the emergence of a transient hexatic state in a TMDC thin-film during the laser-induced transformation between two charge-density wave (CDW) phases. Introducing tilt-series ultrafast nanobeam electron diffraction, we reconstruct CDW rocking curves at high momentum resolution. An intermittent suppression of three-dimensional structural correlations promotes a loss of in-plane translational order characteristic of a hexatic intermediate. Our results demonstrate the merit of tomographic ultrafast structural probing in tracing coupled order parameters, heralding universal nanoscale access to laser-induced dimensionality control in functional heterostructures and devices

Generalized Zero Range Potentials and Multi-Channel Electron-Molecule Scattering

A multi-channel scattering problem is studied from a point of view of integral equations system. The system appears while natural one-particle wave function equation of the electron under action of a potential with non-intersecting ranges is considered. Spherical functions basis expansion of the potentials introduces partial amplitudes and corresponding radial functions. The approach is generalized to multi-channel case by a matrix formulation in which a state vector component is associated with a scattering channel. The zero-range potentials naturally enter the scheme when the class of operators of multiplication is widen to distributions. %Analog of multipolar expansion is treated. Spin variables, o Oscillations and rotations are incorporated into the scheme.Comment: 11 pages, 1 figure, CEPAS2 con

Terahertz control of nanotip photoemission

The active control of matter by strong electromagnetic fields is of growing importance, with applications all across the optical spectrum from the extreme-ultraviolet to the far-infrared. In recent years, phase-stable terahertz fields have shown tremendous potential for observing and manipulating elementary excitations in solids. In the gas phase, on the other hand, driving free charges with terahertz transients provides insight into ultrafast ionization dynamics. Developing such approaches for locally enhanced terahertz fields in nanostructures will create new means to govern electron currents on the nanoscale. Here, we use single-cycle terahertz transients to demonstrate extensive control over nanotip photoelectron emission. The terahertz near-field is shown to either enhance or suppress photocurrents, with the tip acting as an ultrafast rectifying diode6. We record phase-resolved sub-cycle dynamics and find spectral compression and expansion arising from electron propagation within the terahertz near-field. These interactions produce rich spectro-temporal features and offer unprecedented control over ultrashort free electron pulses for imaging and diffraction

A dressing of zero-range potentials and electron-molecule scattering problem at Ramsauer-Townsend minimum

A dressing technique is used to improve zero range potential (ZRP) model. We consider a Darboux transformation starting with a ZRP, the result of the "dressing" gives a potential with non-zero range that depends on a seed solution parameters. Concepts of the partial waves and partial phases for non-spherical potential are used in order to perform Darboux transformation. The problem of scattering on the regular X$_{\hbox{n}}$ and YX$_{\hbox{n}}$ structures is studied. The results of the low-energy electron-molecule scattering on the dressed ZRPs are illustrated by model calculation for the configuration and parameters of the silane ($\hbox{SiH}_4$) molecule. \center{Key words: low-energy scattering, multiple scattering, Ramsauer-Townsend minimum, silane, zero range potential.Comment: 13 pages, 1 figur

Structural dynamics of incommensurate charge-density waves tracked by ultrafast low-energy electron diffraction

We study the non-equilibrium structural dynamics of the incommensurate and nearly commensurate charge-density wave (CDW) phases in 1T-TaS2. Employing ultrafast low-energy electron diffraction with 1 ps temporal resolution, we investigate the ultrafast quench and recovery of the CDW-coupled periodic lattice distortion (PLD). Sequential structural relaxation processes are observed by tracking the intensities of main lattice as well as satellite diffraction peaks and the diffuse scattering background. Comparing distinct groups of diffraction peaks, we disentangle the ultrafast quench of the PLD amplitude from phonon-related reductions of the diffraction intensity. Fluence-dependent relaxation cycles reveal a long-lived partial suppression of the order parameter for up to 60 ps, far outlasting the initial amplitude recovery and electron-phonon scattering times. This delayed return to a quasi-thermal level is controlled by lattice thermalization and coincides with the population of zone-center acoustic modes, as evidenced by a structured diffuse background. The long-lived non-equilibrium order parameter suppression suggests hot populations of CDW-coupled lattice modes. Finally, a broadening of the superlattice peaks is observed at high fluences, pointing to a non-linear generation of phase fluctuation