Photonics and Plasmonics in 4D Ultrafast Electron Microscopy

Light–matter interactions at the nanoscale are fundamental to the rapidly developing fields of plasmonics and nanophotonics. These fields hold the promise of advancing both the speed of computers along with communications and may also provide methods to create a new generation of ultrasensitive molecular biosensors. While there are a variety of techniques that can provide static images of these devices with suboptical wavelength precision there are only a few that are capable of capturing the ultrafast dynamics of electromagnetic fields interacting with or produced by nanomaterials. In this Perspective, we aim to introduce the reader to the newly developed field of 4D ultrafast electron microscopy (4D UEM), which provides a unique window into ultrafast dynamics at the nanoscale. We will describe the basic technique and how internal structural, bulk electronic, and surface near-field dynamics can all be obtained with nanometer and femtosecond resolutions. In addition, we will discuss how a variety of different ultrafast electron microscopes have been used to map the evolution of photonics-related phenomena. Throughout, we discuss the direction of research that will help advance the understanding of light–matter interactions near the atomic scale in both space and time

Femtosecond Photoelectron Point Projection Microscope

By utilizing a nanometer ultrafast electron source in a point projection microscope we demonstrate that images of nanoparticles with spatial resolutions of the order of 100 nanometers can be obtained. The duration of the emission process of the photoemitted electrons used to make images is shown to be of the order of 100 fs using an autocorrelation technique. The compact geometry of this photoelectron point projection microscope does not preclude its use as a simple ultrafast electron microscope, and we use simple analytic models to estimate temporal resolutions that can be expected when using it as a pump-probe ultrafast electron microscope. These models show a significant increase in temporal resolution when comparing to ultrafast electron microscopes based on conventional designs. We also model the microscopes spectroscopic abilities to capture ultrafast phenomena such as the photon induced near field effect

Design and implementation of a fs-resolved transmission electron microscope based on thermionic gun technology [post-print]

In this paper, the design and implementation of a femtosecond-resolved ultrafast transmission electron microscope is presented, based on a thermionic gun geometry. Utilizing an additional magnetic lens between the electron acceleration and the nominal condenser lens system, a larger percentage of the electrons created at the cathode are delivered to the specimen without degrading temporal, spatial and energy resolution significantly, while at the same time maintaining the femtosecond temporal resolution. Using the photon-induced near field electron microscopy effect (PINEM) on silver nanowires the cross-correlation between the light and electron pulses was measured, showing the impact of the gun settings and initiating laser pulse duration on the electron bunch properties. Tuneable electron pulses between 300 fs and several ps can be obtained, and an overall energy resolution around 1 eV was achieved

Shaping, imaging and controlling plasmonic interference fields at buried interfaces

Filming and controlling plasmons at buried interfaces with nanometer (nm) and femtosecond (fs) resolution has yet to be achieved and is critical for next generation plasmonic/electronic devices. In this work, we use light to excite and shape a plasmonic interference pattern at a buried metal-dielectric interface in a nanostructured thin film. Plasmons are launched from a photoexcited array of nanocavities and their propagation is filmed via photon-induced near-field electron microscopy (PINEM). The resulting movie directly captures the plasmon dynamics, allowing quantification of their group velocity at approximately 0.3c, consistent with our theoretical predictions. Furthermore, we show that the light polarization and nanocavity design can be tailored to shape transient plasmonic gratings at the nanoscale. These results, demonstrating dynamical imaging with PINEM, pave the way for the fs/nm visualization and control of plasmonic fields in advanced heterostructures based on novel 2D materials such as graphene, MoS$_2$, and ultrathin metal films.Comment: 16 pages, 5 figures, 3 supplementary figure

Photon-induced near-field electron microscopy

In materials science and biology, optical near-field microscopies enable spatial resolutions beyond the diffraction limit, but they cannot provide the atomic-scale imaging capabilities of electron microscopy. Given the nature of interactions between electrons and photons, and considering their connections through nanostructures, it should be possible to achieve imaging of evanescent electromagnetic fields with electron pulses when such fields are resolved in both space (nanometre and below) and time (femtosecond). Here we report the development of photon-induced near-field electron microscopy (PINEM), and the associated phenomena. We show that the precise spatiotemporal overlap of femtosecond single-electron packets with intense optical pulses at a nanostructure (individual carbon nanotube or silver nanowire in this instance) results in the direct absorption of integer multiples of photon quanta (nħω) by the relativistic electrons accelerated to 200 keV. By energy-filtering only those electrons resulting from this absorption, it is possible to image directly in space the near-field electric field distribution, obtain the temporal behaviour of the field on the femtosecond timescale, and map its spatial polarization dependence. We believe that the observation of the photon-induced near-field effect in ultrafast electron microscopy demonstrates the potential for many applications, including those of direct space-time imaging of localized fields at interfaces and visualization of phenomena related to photonics, plasmonics and nanostructures

Laser-induced ultrafast electron emission from a field emission tip

We show that a field emission tip electron source that is triggered with a femtosecond laser pulse can generate electron pulses shorter than the laser pulse duration (100&#; fs). The emission process is sensitive to a power law of the laser intensity, which supports an emission mechanism based on multiphoton absorption followed by over-the-barrier emission. Observed continuous transitions between power laws of different orders are indicative of field emission processes. We show that the source can also be operated so that thermionic emission processes become significant. Understanding these different emission processes is relevant for the production of sub-cycle electron pulses

4D imaging of transient structures and morphologies in ultrafast electron microscopy

With advances in spatial resolution reaching the atomic scale, two-dimensional (2D) and 3D imaging in electron microscopy has become an essential methodology in various fields of study. Here, we report 4D imaging, with in situ spatiotemporal resolutions, in ultrafast electron microscopy (UEM). The ability to capture selected-area-image dynamics with pixel resolution and to control the time separation between pulses for temporal cooling of the specimen made possible studies of fleeting structures and morphologies. We demonstrate the potential for applications with two examples, gold and graphite. For gold, after thermally induced stress, we determined the atomic structural expansion, the nonthermal lattice temperature, and the ultrafast transients of warping/bulging. In contrast, in graphite, striking coherent transients of the structure were observed in both image and diffraction, directly measuring, on the nanoscale, the longitudinal resonance period governed by Young's elastic modulus. The success of these studies demonstrates the promise of UEM in real-space imaging of dynamics