Influence of Discrete Defects on Observed Acoustic-Phonon Dynamics in Layered Materials Probed with Ultrafast Electron Microscopy.

The structural anisotropy of layered materials leads to disparate lattice responses along different crystallographic directions following femtosecond photoexcitation. Ultrafast scattering methods are well-suited to resolving such responses, though probe size and specimen structure and morphology must be considered when interpreting results. Here we use ultrafast electron microscopy (UEM) imaging and diffraction to study the influence of individual multilayer terraces and few-layer step-edges on acoustic-phonon dynamics in 1T-TaS2 and 2H-MoS2. In TaS2, we find that a multilayer terrace produces distinct, localized responses arising from thickness-dependent c-axis phonon dynamics. Convolution of the responses is demonstrated with ultrafast selected-area diffraction by limiting the probe size and training it on the region of interest. This results in a reciprocal-space frequency response that is a convolution of the spatially separated behaviors. Sensitivity of phonon dynamics to few-layer step-edges in MoS2 and the capability of UEM imaging to resolve the influence of such defects are also demonstrated. Spatial frequency maps from the UEM image series reveal regions separated by a four-layer step-edge having 60.0 GHz and 63.3 GHz oscillation frequencies, again linked to c-axis phonon propagation. As with ultrafast diffraction, signal convolution is demonstrated by continuous increase of the size of the selected region of interest used in the analysis.

Characterization of transverse electron pulse trains using RF powered traveling wave metallic comb striplines.

Advancements in ultrafast electron microscopy have allowed elucidation of spatially selective structural dynamics. However, as the spatial resolution and imaging capabilities have made progress, quantitative characterization of the electron pulse trains has not been reported at the same rate. In fact, inexperienced users have difficulty replicating the technique because only a few dedicated microscopes have been characterized thoroughly. Systems replacing laser driven photoexcitation with electrically driven deflectors especially suffer from a lack of quantified characterization because of the limited quantity. The primary advantages to electrically driven systems are broader frequency ranges, ease of use and simple synchronization to electrical pumping. Here, we characterize the technical parameters for electrically driven UEM including the shape, size and duration of the electron pulses using low and high frequency chopping methods. At high frequencies, pulses are generated by sweeping the electron beam across a chopping aperture. For low frequencies, the beam is continuously forced off the optic axis by a DC potential, then momentarily aligned by a countering pulse. Using both methods, we present examples that measure probe durations of 2 ns and 10 ps for the low and high frequency techniques, respectively. We also discuss how the implementation of a pulsed probe affects STEM imaging conditions by adjusting the first condenser lens.

Stroboscopic ultrafast imaging using RF strip-lines in a commercial transmission electron microscope.

The development of ultrafast electron microscopy (UEM), specifically stroboscopic imaging, has brought the study of structural dynamics to a new level by overcoming the spatial limitations of ultrafast spectroscopy and the temporal restrictions of traditional TEM simultaneously. Combining the concepts governing both techniques has enabled direct visualization of dynamics with spatiotemporal resolutions in the picosecond-nanometer regime. Here, we push the limits of imaging using a pulsed electron beam via RF induced transverse deflection based on the newly developed 200 keV frequency-tunable strip-line pulser. We demonstrate a 0.2 nm spatial resolution and elucidation of magnetic spin induction maps using the phase-microscopy method. We also present beam coherence measurements and expand our study using the breathing modes of a silicon interdigitated comb under RF excitation which achieves improved temporal synchronization between the electron pulse-train and electric field. A new RF holder has also been developed with impedance matching to the RF signal to minimize transmission power loss to samples and its performance is compared with a conventional sample holder.

UEMtomaton: A Source-Available Platform to Aid in Start-up of Ultrafast Electron Microscopy Labs.

The steady rise in the number of ultrafast electron microscopy (UEM) labs, in addition to the opacity and lack of detailed descriptions of current approaches that would enable point-by-point construction, has created an opportunity for sharing common methods and instrumentation for (for example) automating data acquisition to assist in efficient lab start-up and to learn about common and robust protocols. In the spirit of open sharing of methods, we provide here a description of an entry-level method and user interface (UI) for automating UEM experiments, and we provide access to the source code and scripts (source-available) for ease of implementation or as a starting reference point for those entering or seeking to enter the field (https://github.com/CEMSFlannigan/UEMtomaton/releases/tag/v1.0). Core instrumentation and physical connections in the UEM lab at Minnesota are described. Interface communication schemes consisting of duo server-client pairs between critical components - the optical delay stage and the UEM digital camera - are presented, with emphasis placed on describing the logic and communications sequence designed to conduct automated series acquisitions. An application designed and programmed with C++/CLI as Windows Forms in Microsoft Visual Studio - dubbed UEMtomaton - is also presented. Key to the UI layout is centralization of the automation tasks and establishment of communication within the software rather than by interfacing with each individual workstation. It is our hope that this note provides useful insight for current and future UEM researchers, particularly with respect to generalizability and portability of the approach to emerging labs. We note that while this basic, entry-level approach is certainly not the most sophisticated or comprehensive of those currently in use, we feel there is nevertheless value in clearly communicating a proven straightforward method to hopefully lower the barrier to entry into the field.

Coherent Phonon Disruption and Lock-In during a Photoinduced Charge-Density-Wave Phase Transition.

Ultrafast manipulation of phase domains in quantum materials is a promising approach to unraveling and harnessing interwoven charge and lattice degrees of freedom. Here we find evidence for coupling of displacively excited coherent acoustic phonons (CAPs) and periodic lattice distortions (PLDs) in the intensely studied charge-density-wave material, 1T-TaS2, using 4D ultrafast electron microscopy (UEM). Initial photoinduced Bragg-peak dynamics reveal partial CAP coherence and localized c-axis dilations. Weak, partially coherent dynamics give way to higher-amplitude, increasingly coherent oscillations, the transition period of which matches that of photoinduced incommensurate domain growth and stabilization from the nearly-commensurate phase. With UEM imaging, it is found that phonon wave trains emerge from linear defects 100 ps after photoexcitation. The CAPs consist of coupled longitudinal and transverse character and propagate at anomalously high velocities along wave vectors independent from PLDs, instead being dictated by defect orientation. Such behaviors illustrate a means to control phases in quantum materials using defect-engineered coherent-phonon seeding.