Lossless Monochromator in an Ultrafast Electron Microscope Using Near-Field THz Radiation.

The ability to form monoenergetic electron beams is vital for high-resolution electron spectroscopy and imaging. Such capabilities are commonly achieved using an electron monochromator, which energy filters a dispersed electron beam, thus reducing the electron flux to yield down to meV energy resolution. This reduction in flux hinders the use of monochromators in many applications, such as ultrafast transmission electron microscopes (UTEMs). Here, we develop and demonstrate a mechanism for electron energy monochromation that does not reduce the flux-a lossless monochromator. The mechanism is based on the interaction of free-electron pulses with single-cycle THz near fields, created by nonlinear conversion of an optical laser pulse near the electron beam path inside a UTEM. Our experiment reduces the electron energy spread by a factor of up to 2.9 without compromising the beam flux. Moreover, as the electron-THz interaction takes place over an extended region of many tens of microns in free space, the realized technique is highly robust-granting uniform monochromation over a wide area, larger than the electron beam diameter. We further demonstrate the wide tunability of our method by monochromating the electron beam at multiple primary electron energies from 60 to 200 keV, studying the effect of various electron and THz parameters on its performance. Our findings have direct applications in the fast-growing field of ultrafast electron microscopy, allowing time- and energy-resolved studies of exciton physics, phononic vibrational resonances, charge transport effects, and optical excitations in the mid IR to the far IR.

Generation and control of localized terahertz fields in photoemitted electron plasmas.

Dense micron-sized electron plasmas, such as those generated upon irradiation of nanostructured metallic surfaces by intense femtosecond laser pulses, constitute a rich playground to study light-matter interactions, many-body phenomena, and out-of-equilibrium charge dynamics. Besides their fundamental interest, laser-induced plasmas hold great potential for the generation of localized terahertz radiation pulses. However, the underlying mechanisms ruling the formation and evolution of such plasmas are not yet well understood. Here, we develop a comprehensive microscopic theory to predictably describe the spatiotemporal dynamics of laser-pulse-induced plasmas. Through detailed analysis of electron emission, metal screening, and plasma cloud interactions, we investigate the spatial, temporal, and spectral characteristics of the so-generated terahertz fields, which can be extensively controlled through the metal morphology and the illumination conditions. We further describe the interaction with femtosecond electron beams to explain recent ultrafast electron microscopy experiments, whereby the position and temporal dependence of the observed electron acceleration permits assessing the associated terahertz field. Besides its potential application to the design of low-frequency light sources, our work contributes fundamental insight into the generation and dynamics of micron-scale electron plasmas and their interaction with ultrafast electron pulses.

Imaging the field inside nanophotonic accelerators.

Controlling optical fields on the subwavelength scale is at the core of nanophotonics. Laser-driven nanophotonic particle accelerators promise a compact alternative to conventional radiofrequency-based accelerators. Efficient electron acceleration in nanophotonic devices critically depends on achieving nanometer control of the internal optical nearfield. However, these nearfields have so far been inaccessible due to the complexity of the devices and their geometrical constraints, hampering the design of future nanophotonic accelerators. Here we image the field distribution inside a nanophotonic accelerator, for which we developed a technique for frequency-tunable deep-subwavelength resolution of nearfields based on photon-induced nearfield electron-microscopy. Our experiments, complemented by 3D simulations, unveil surprising deviations in two leading nanophotonic accelerator designs, showing complex field distributions related to intricate 3D features in the device and its fabrication tolerances. We envision an extension of our method for full 3D field tomography, which is key for the future design of highly efficient nanophotonic devices.

Charge Dynamics Electron Microscopy: Nanoscale Imaging of Femtosecond Plasma Dynamics.

Understanding and actively controlling the spatiotemporal dynamics of nonequilibrium electron clouds is fundamental for the design of light and electron sources, high-power electronic devices, and plasma-based applications. However, electron clouds evolve in a complex collective fashion on the nanometer and femtosecond scales, producing electromagnetic screening that renders them inaccessible to existing optical probes. Here, we solve the long-standing challenge of characterizing the evolution of electron clouds generated upon irradiation of metallic structures using an ultrafast transmission electron microscope to record the charged plasma dynamics. Our approach to charge dynamics electron microscopy (CDEM) is based on the simultaneous detection of electron-beam acceleration and broadening with nanometer/femtosecond resolution. By combining experimental results with comprehensive microscopic theory, we provide a deep understanding of this highly out-of-equilibrium regime, including previously inaccessible intricate microscopic mechanisms of electron emission, screening by the metal, and collective cloud dynamics. Beyond the present specific demonstration, the here-introduced CDEM technique grants us access to a wide range of nonequilibrium electrodynamic phenomena involving the ultrafast evolution of bound and free charges on the nanoscale.

Ultrafast Electron Microscopy of Nanoscale Charge Dynamics in Semiconductors.

The ultrafast dynamics of charge carriers in solids plays a pivotal role in emerging optoelectronics, photonics, energy harvesting, and quantum technology applications. However, the investigation and direct visualization of such nonequilibrium phenomena remains as a long-standing challenge, owing to the nanometer-femtosecond spatiotemporal scales at which the charge carriers evolve. Here, we propose and demonstrate an interaction mechanism enabling nanoscale imaging of the femtosecond dynamics of charge carriers in solids. This imaging modality, which we name charge dynamics electron microscopy (CDEM), exploits the strong interaction of free-electron pulses with terahertz (THz) near fields produced by the moving charges in an ultrafast scanning transmission electron microscope. The measured free-electron energy at different spatiotemporal coordinates allows us to directly retrieve the THz near-field amplitude and phase, from which we reconstruct movies of the generated charges by comparison to microscopic theory. The CDEM technique thus allows us to investigate previously inaccessible spatiotemporal regimes of charge dynamics in solids, providing insight into the photo-Dember effect and showing oscillations of photogenerated electron-hole distributions inside a semiconductor. Our work facilitates the exploration of a wide range of previously inaccessible charge-transport phenomena in condensed matter using ultrafast electron microscopy.

Spatiotemporal imaging of 2D polariton wave packet dynamics using free electrons.

Coherent optical excitations in two-dimensional (2D) materials, 2D polaritons, can generate a plethora of optical phenomena that arise from the extraordinary dispersion relations that do not exist in regular materials. Probing of the dynamical phenomena of 2D polaritons requires simultaneous spatial and temporal imaging capabilities and could reveal unknown coherent optical phenomena in 2D materials. Here, we present a spatiotemporal measurement of 2D wave packet dynamics, from its formation to its decay, using an ultrafast transmission electron microscope driven by femtosecond midinfrared pulses. The ability to coherently excite phonon-polariton wave packets and probe their evolution in a nondestructive manner reveals intriguing dispersion-dependent dynamics that includes splitting of multibranch wave packets and, unexpectedly, wave packet deceleration and acceleration. Having access to the full spatiotemporal dynamics of 2D wave packets can be used to illuminate puzzles in topological polaritons and discover exotic nonlinear optical phenomena in 2D materials.

Photonic Topological Spin Hall Effect Mediated by Vortex Pairs.

Over the past decades, topology has provided unique insight into numerous physical phenomena. Here, we report on a topological mechanism for spin-dependent photonic transport. We observe photonic topological defects of bound vortex pairs and unbound vortices generated from a two-dimensional array of nanoantennas, i.e., a metasurface, which is achieved by randomly inserting local deformations in the metasurfaces, inducing the Pancharatnam-Berry phase. The observed spin-dependent bound vortex pairs are established as the origin of the photonic topological spin Hall effect-a subdiffraction-limited spin-split mode in momentum space, while the spin-dependent unbound vortices induce random spin-split modes throughout the entire momentum space as a random Rashba effect. The topological phenomena-creation of bound vortex pairs and unbound vortices-indicate the universality of the topological effect for particles of different natures.

Spectrally interleaved topologies using geometric phase metasurfaces.

Metasurfaces facilitate the interleaving of multiple topologies in an ultra-thin photonic system. Here, we report on the spectral interleaving of topological states of light using a geometric phase metasurface. We realize that a dielectric spectrally interleaved metasurface generates multiple interleaved vortex beams at different wavelengths. By harnessing the space-variant polarization manipulations that are enabled by the geometric phase mechanism, a vectorial vortex array is implemented. The presented interleaved topologies concept can greatly enhance the functionality of advanced microscopy and communication systems.

Disorder-induced optical transition from spin Hall to random Rashba effect.

Disordered structures give rise to intriguing phenomena owing to the complex nature of their interaction with light. We report on photonic spin-symmetry breaking and unexpected spin-optical transport phenomena arising from subwavelength-scale disordered geometric phase structure. Weak disorder induces a photonic spin Hall effect, observed via quantum weak measurements, whereas strong disorder leads to spin-split modes in momentum space, a random optical Rashba effect. Study of the momentum space entropy reveals an optical transition upon reaching a critical point where the structure's anisotropy axis vanishes. Incorporation of singular topology into the disordered structure demonstrates repulsive vortex interaction depending on the disorder strength. The photonic disordered geometric phase can serve as a platform for the study of different phenomena emerging from complex media involving spin-orbit coupling.

Multifunctional interleaved geometric-phase dielectric metasurfaces.

Shared-aperture technology for multifunctional planar systems, performing several simultaneous tasks, was first introduced in the field of radar antennas. In photonics, effective control of the electromagnetic response can be achieved by a geometric-phase mechanism implemented within a metasurface, enabling spin-controlled phase modulation. The synthesis of the shared-aperture and geometric-phase concepts facilitates the generation of multifunctional metasurfaces. Here shared-aperture geometric-phase metasurfaces were realized via the interleaving of sparse antenna sub-arrays, forming Si-based devices consisting of multiplexed geometric-phase profiles. We study the performance limitations of interleaved nanoantenna arrays by means of a Wigner phase-space distribution to establish the ultimate information capacity of a metasurface-based photonic system. Within these limitations, we present multifunctional spin-dependent dielectric metasurfaces, and demonstrate multiple-beam technology for optical rotation sensing. We also demonstrate the possibility of achieving complete real-time control and measurement of the fundamental, intrinsic properties of light, including frequency, polarization and orbital angular momentum.