Tunable photon-induced spatial modulation of free electrons

Spatial modulation of electron beams is an essential tool for various applications such as nanolithography and imaging, yet its implementations are severely limited and inherently non-tunable. Conversely, light-driven electron spatial modulation could potentially allow arbitrary electron wavefront shaping via the underlying mechanism of photon-induced near-field electron microscopy (PINEM). Here, we present tunable photon-induced spatial modulation of electrons through their externally-controlled interaction with surface plasmon polaritons (SPPs). Using recently developed methods of shaping SPP patterns, we demonstrate a dynamic control of the electron beam with a variety of high-quality electron distributions. Intriguingly, by utilizing the intrinsic interaction nonlinearity, we attain the first observation of 2D spatial Rabi oscillations and generate electron features below the SPP wavelength. Our work paves the way to on-demand electron wavefront shaping at ultrafast timescales, with prospects for aberration correction, nano-fabrication and material characterization

Coherent interaction between free electrons and a photonic cavity

Since its inception, research of cavity quantum electrodynamics (CQED) has extended our understanding of light-matter interactions and our ability to utilize them. Thus far, all the work in this field has been focused on light interacting with bound electron systems - such as atoms, molecules, quantum dots, and quantum circuits. In contrast, markedly different physical phenomena are found in free-electron systems, the energy distribution of which is continuous and not discrete, implying tunable transitions and selection rules. In addition to their uses for electron microscopy, the interaction of free electrons with light enables important phenomena such as Cherenkov radiation, Compton scattering, and free-electron lasing. However, no experiment has shown the integration of free electrons into the framework of CQED, because the fundamental electron-light interaction is limited in strength and lifetime. This limit explains why many phenomena have remained out of reach for experiments with free electrons. In this work, we developed the platform for studying CQED at the nanoscale with free electrons and demonstrated it by observing their coherent interaction with cavity photons for the first time. We also directly measure the cavity photon lifetime via a free electron probe and show more than an order of magnitude enhancement in the electron-photon interaction strength. These capabilities may open new paths toward using free electrons as carriers of quantum information, even more so after strong coupling between free electrons and cavity photons will have been demonstrated. Efficient electron-cavity photon coupling could also allow new nonlinear phenomena of cavity opto-electro-mechanics and the ultrafast exploration of soft matter or other beam-sensitive materials using low electron current and low laser exposure

Observation of 2D Cherenkov radiation

For over 80 years of research, the conventional description of free-electron radiation phenomena, such as Cherenkov radiation, has remained unchanged: classical three-dimensional electromagnetic waves. Interestingly, in reduced dimensionality, the properties of free-electron radiation are predicted to fundamentally change. Here, we present the first observation of Cherenkov surface waves, wherein free electrons emit narrow-bandwidth photonic quasiparticles propagating in two-dimensions. The low dimensionality and narrow bandwidth of the effect enable to identify quantized emission events through electron energy loss spectroscopy. Our results support the recent theoretical prediction that free electrons do not always emit classical light and can instead become entangled with the photons they emit. The two-dimensional Cherenkov interaction achieves quantum coupling strengths over two orders of magnitude larger than ever reported, reaching the single-electron-single-photon interaction regime for the first time with free electrons. Our findings pave the way to previously unexplored phenomena in free-electron quantum optics, facilitating bright, free-electron-based quantum emitters of heralded Fock states

Ultrafast Nonlinear Excitation Dynamics of Black Phosphorus Nanosheets from Visible to Mid-Infrared

The recent progress on black phosphorus makes it a promising candidate material for broadband nanophotonic devices, especially operating in the mid-infrared spectral region. Here, the excited carrier dynamics and nonlinear optical response of unoxidized black phosphorus nanosheets and their wavelength dependence were systematically studied from 800 nm to 2.1 μm. The wavelength-dependent relaxation times of black phosphorus nanosheets are determined to be 360 fs to 1.36 ps with photon energies from 1.55 to 0.61 eV. In a comparative study with graphene, we found that black phosphorus has a faster carrier relaxation in near- and mid-infrared region. With regard to nonlinear optical absorption, the response of black phosphorus significantly increases from near- to mid-infrared, and black phosphorus is also confirmed to be better as saturable absorber to MoS₂ in infrared region

Observation of the Stimulated Quantum Cherenkov Effect

As charged particles surpass the speed of light in an optical medium they produce radiation - analogously to the way jet planes surpass the speed of sound and produce a sonic boom. This radiation emission, known as the Cherenkov effect, is among the most fundamental processes in electrodynamics. As such, it is used in numerous applications of particle detectors, particle accelerators, light sources, and medical imaging. Surprisingly, all Cherenkov-based applications and experiments thus far were fully described by classical electrodynamics even though theoretical work predicts new Cherenkov phenomena coming from quantum electrodynamics. The quantum description could provide new possibilities for the design of highly controllable light sources and more efficient accelerators and detectors. Here, we provide a direct evidence of the quantum nature of the Cherenkov effect and reveal its intrinsic quantum features. By satisfying the Cherenkov condition for relativistic electron wavefunctions and maintaining it over hundreds of microns, each electron simultaneously accelerates and decelerates by absorbing and emitting hundreds of photons in a coherent manner. We observe this strong interaction in an ultrafast transmission electron microscope, achieving for the first time a phase-matching between a relativistic electron wavefunction and a propagating light wave. Consequently, the quantum wavefunction of each electron evolves into a coherent plateau, analogous to a frequency comb in ultrashort laser pulses, containing hundreds of quantized energy peaks. Our findings prove that the delocalized wave nature of electrons can become dominant in stimulated interactions. In addition to prospects for known applications of the Cherenkov effect, our work provides a platform for utilizing quantum electrodynamics for applications in electron microscopy and in free-electron pump-probe spectroscopy

Demonstration of weak measurements, projective measurements, and quantum-to-classical transitions in ultrafast free electron-photon interactions

How does the quantum-to-classical transition of measurement occur? This question is vital for both foundations and applications of quantum mechanics. Here, we develop a new measurement-based framework for characterizing the classical and quantum free electron-photon interactions and then experimentally test it. We first analyze the transition from projective to weak measurement in generic light-matter interactions and show that any classical electron-laser-beam interaction can be represented as an outcome of a weak measurement. In particular, the appearance of classical point-particle acceleration is an example of an amplified weak value resulting from weak measurement. A universal factor quantifies the measurement regimes and their transition from quantum to classical, where Gamma corresponds to the ratio between the electron wavepacket size and the optical wavelength. This measurement-based formulation is experimentally verified in both limits of photon-induced near-field electron microscopy and the classical acceleration regime using a dielectric laser accelerator. Our results shed new light on the transition from quantum to classical electrodynamics, enabling to employ the essence of wave-particle duality of both light and electrons in quantum measurement for exploring and applying many quantum and classical light-matter interactions

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

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

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

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