Photoemission electron microscopy was used to image the electrons photoemitted from specially tailored Ag nanoparticles deposited on a Si substrate (with its native oxide SiO$_{x}$). Photoemission was induced by illumination with a Hg UV-lamp (photon energy cutoff $\hbarω_{UV}=5.0$ eV, wavelength $λ_{UV}=250$ nm) and with a Ti:Sapphire femtosecond laser ($\hbarω_{l}=3.1$ eV, $λ_{l}=400$ nm, pulse width below 200 fs), respectively. While homogeneous photoelectron emission from the metal is observed upon illumination at energies above the silver plasmon frequency, at lower photon energies the emission is localized at tips of the structure. This is interpreted as a signature of the local electrical field therefore providing a tool to map the optical near field with the resolution of emission electron microscopy.
We report on the investigation of an advanced circular plasmonic nanoantenna under ultrafast excitation using nonlinear photoemission electron microscopy (PEEM) under near-normal incidence. The circular nanoantenna is enhanced in its performance by a supporting grating and milled out from a gold film. The considered antenna shows a sophisticated physical resonance behavior that is ideal to demonstrate the possibilities of PEEM for the experimental investigations of plasmonic effects on the nanoscale. Field profiles of the antenna resonance for both possible linear polarizations of the incident…
We image the field enhancement at Ag nanostructures using femtosecond laser pulses with a center wavelength of 1.55 micrometer. Imaging is based on non-linear photoemission observed in a photoemission electron microscope (PEEM). The images are directly compared to ultra violet PEEM and scanning electron microscopy (SEM) imaging of the same structures. Further, we have carried out atomic scale scanning tunneling microscopy (STM) on the same type of Ag nanostructures and on the Au substrate. Measuring the photoelectron spectrum from individual Ag particles shows a larger contribution from higher…
Femtosecond point-projection microscopy (fs-PPM) is an electron microscopy technique that possesses a combination of high spatio-temporal resolution and sensitivity to local electric fields. This allows it to visualize ultrafast charge carrier dynamics in complex nanomaterials. We benchmark the capability of the fs-PPM technique by imaging the ultrafast dynamics of charge carriers produced by multiphoton ionization of silver nanowires. The space-charge driven motion of photoelectrons is followed on \mbox{sub-100}\,nm length scales, while the dynamics are captured on 30-100 fs time scales. The …
With rapidly growing photoconversion efficiencies, hybrid perovskite solar cells have emerged as promising contenders for next generation, low-cost photovoltaic technologies. Yet, the presence of nanoscale defect clusters, that form during the fabrication process, remains critical to overall device operation, including efficiency and long-term stability. To successfully deploy hybrid perovskites, we must understand the nature of the different types of defects, assess their potentially varied roles in device performance, and understand how they respond to passivation strategies. Here, by correl…
Watching the motion of electrons on their natural nanometre length- and femtosecond time scales is a fundamental goal and an open challenge of contemporary ultrafast science. Optical techniques and electron microscopy currently mostly provide either ultrahigh temporal or spatial resolution, yet, microscopy techniques with combined space-time resolution need further development. Here we create an ultrafast electron source by plasmon nanofocusing on a sharp gold taper and implement this source in an ultrafast point-projection electron microscope. This source is used, in an optical pump - electro…
Transient near-fields around metallic nanotips drive many applications, including the generation of ultrafast electron pulses and their use in electron microscopy. We have investigated the electron emission from a gold nanotip driven by mid-infrared few-cycle laser pulses. We identify a low-energy peak in the kinetic energy spectrum and study its shift to higher energies with increasing laser intensities from $1.7$ to $3.7\cdot10^{11} \mathrm{W}/\mathrm{cm}^2$. The experimental observation of the upshift of the low-energy peak is compared to a simple model and numerical simulations, which show…
Given the quasi-static nature of optical-field emission and the nontrivial dependence of the emission rate on the instantaneous electric field strength, the CEP-sensitive component of the emitted photocurrent is highly sensitive to the energy of the optical pulse, and should carry information about the underlying sub-cycle dynamics of electron emission. Here we examine CEP-sensitive photoemission from plasmonic gold nanoantennas excited with few-cycle optical pulses of increasing energy. We observe antiresonance-like features in the CEP-sensitive photocurrent; specifically, at a critical pulse…
Ultrafast electron pulses, combined with laser-pump and electron-probe technologies, allow for various forms of ultrafast microscopy and spectroscopy to elucidate otherwise challenging to observe physical and chemical transitions. However, the pursuit of simultaneous ultimate spatial and temporal resolution has been largely subdued by the low monochromaticity of the electron pulses and their poor phase synchronization to the optical excitation pulses. State-of-the-art photon-driven sources have good monochromaticity but poor phase synchronization. In contrast, field-driven photoemission has mu…
Many optical approaches have been used to examine the composition and structure of gemstones, both recently and throughout history. The nonlinear optical behavior of different gemstones has not been investigated, and the higher order terms to the refractive index represent an unused tool for qualifying and examining a stone. We have used a multiphoton microscope to examine the nonlinear optical properties of 36 different gemstones and demonstrate that it is a useful tool for imaging them three-dimensionally up to the millimeter scale below the sample surface. The polarization dependence of sec…
Momentum microscopy of ultrafast electron emission from a strongly driven optical nanoantenna
Carl von Ossietzky Universität Oldenburg（奥尔登堡卡尔·冯·奥西茨基大学）；ELI ALPS, The Extreme Light Infrastructure ERIC（ELI ALPS，极端光基础设施ERIC）；Leibniz Institute of Photonic Technology（莱布尼兹光子技术研究所）；Universität Würzburg（维尔茨堡大学）；Friedrich-Schiller-Universität Jena（耶拿弗里德里希·席勒大学）；HUN-REN Wigner Research Center for Physics（匈牙利科学院Wigner物理研究中心）
Super-resolution optical microscopy is a rapidly evolving scientific field dedicated to imaging sub-wavelength sized objects, leaving its mark in multiple branches of biology and technology. While several super-resolution optical microscopy methods have become a common tool in life science imaging, new methods, supported by cutting-edge technology, continue to emerge. One rather recent addition to the super-resolution toolbox, image scanning microscopy (ISM), achieves an up to twofold lateral resolution enhancement in a robust and straightforward manner. To further enhance ISM's resolution in …
We derive the fundamental limit to the resolution of far-field optical imaging, and demonstrate that, while a bound to the resolution of a fundamental nature does exit, contrary to the conventional wisdom it is neither exactly equal to nor necessarily close to Abbe's estimate. Our approach to imaging resolution that combines the tools from the physics of wave phenomena and the methods of information theory, is general, and can be extended beyond optical microscopy, to e.g. geophysical and ultrasound imaging.
The role and importance of mechanical properties of cells and tissues in cellular function, development as well as disease has widely been acknowledged, however standard techniques currently used to assess them exhibit intrinsic limitations. Recently, a new type of optical elastography, namely Brillouin microscopy, has emerged as a non-destructive, label- and contact-free method which can probe the viscoelastic properties of biological samples with diffraction-limited resolution in 3D. This has led to increased attention amongst the biological and medical research communities, but also to deba…
Understanding and controlling ultrafast non-equilibrium charge carrier dynamics is of fundamental importance in diverse fields of (quantum) science and technology. Here, we create a three-dimensional hot electron gas through two-photon photoemission from a copper surface in vacuum. We employ an ultrafast electron microscope to record movies of the subsequent electron dynamics on the picosecond-nanosecond time scale. After a prompt Coulomb explosion, the subsequent dynamics is characterized by a rapid oblate-to-prolate shape transformation of the electron gas, and exceptionally periodic and lon…
We present a novel experimental setup in which magnetic and optical tweezers are combined for torque and force transduction onto single filamentous molecules in a transverse configuration to allow simultaneous mechanical measurement and manipulation. Previously we have developed a super-resolution imaging module which in conjunction with advanced imaging techniques such as Blinking assisted Localisation Microscopy (BaLM) achieves localisation precision of single fluorescent dye molecules bound to DNA of ~30 nm along the contour of the molecule; our work here describes developments in producing…
