Towards attosecond 4D imaging of atomic-scale dynamics by single-electron diffraction

Many physical and chemical processes which define our daily life take place on atomic scales in space and time. Time-resolved electron diffraction is an excellent tool for investigation of atomic-scale structural dynamics (4D imaging) due to the short de Broglie wavelength of fast electrons. This requires electron pulses with durations on the order of femtoseconds or below. Challenges arise from Coulomb repulsion and dispersion of non-relativistic electron wave packets in vacuum, which currently limits the temporal resolution of diffraction experiments to some hundreds of femtoseconds. In order to eventually advance the temporal resolution of electron diffraction into the few-femtosecond range or below, four new concepts are investigated and combined in this work: First, Coulomb repulsion is avoided by using only a single electron per pulse, which does not repel itself but interferes with itself when being diffracted from atoms. Secondly, dispersion control for electron pulses is implemented with time-dependent electric fields at microwave frequencies, compressing the duration of single-electron pulses at the expense of simultaneous energy broadening. Thirdly, a microwave signal used for electron pulse compression is derived from an ultrashort laser pulse train. Optical enhancement allows a temporal synchronization between the microwave field and the laser pulses with a precision below one femtosecond. Fourthly, a cross-correlation between laser and electron pulses is measured in this work with the purpose of determining the possible temporal resolution of diffraction experiments employing compressed single-electron pulses. This novel characterization method uses the principles of a streak camera with optical fields and potentially offers attosecond temporal resolution. These four concepts show a clear path towards improving the temporal resolution of electron diffraction into the few-femtosecond domain or below, which opens the possibility of observing electron densities in motion. In this work, a compressed electron pulse's duration of 28±5 fs full width at half maximum (12±2 fs standard deviation) at a de Broglie wavelength of 0.08 Å is achieved. Currently, this constitutes the shortest electron pulses suitable for diffraction, about sixfold shorter than in previous work. Ultrafast electron diffraction now meets the requirements for investigating the fastest primary processes in molecules and solids with atomic resolution in space and time

Towards attosecond 4D imaging of atomic-scale dynamics by single-electron diffraction

Many physical and chemical processes which define our daily life take place on atomic scales in space and time. Time-resolved electron diffraction is an excellent tool for investigation of atomic-scale structural dynamics (4D imaging) due to the short de Broglie wavelength of fast electrons. This requires electron pulses with durations on the order of femtoseconds or below. Challenges arise from Coulomb repulsion and dispersion of non-relativistic electron wave packets in vacuum, which currently limits the temporal resolution of diffraction experiments to some hundreds of femtoseconds. In order to eventually advance the temporal resolution of electron diffraction into the few-femtosecond range or below, four new concepts are investigated and combined in this work: First, Coulomb repulsion is avoided by using only a single electron per pulse, which does not repel itself but interferes with itself when being diffracted from atoms. Secondly, dispersion control for electron pulses is implemented with time-dependent electric fields at microwave frequencies, compressing the duration of single-electron pulses at the expense of simultaneous energy broadening. Thirdly, a microwave signal used for electron pulse compression is derived from an ultrashort laser pulse train. Optical enhancement allows a temporal synchronization between the microwave field and the laser pulses with a precision below one femtosecond. Fourthly, a cross-correlation between laser and electron pulses is measured in this work with the purpose of determining the possible temporal resolution of diffraction experiments employing compressed single-electron pulses. This novel characterization method uses the principles of a streak camera with optical fields and potentially offers attosecond temporal resolution. These four concepts show a clear path towards improving the temporal resolution of electron diffraction into the few-femtosecond domain or below, which opens the possibility of observing electron densities in motion. In this work, a compressed electron pulse's duration of 28±5 fs full width at half maximum (12±2 fs standard deviation) at a de Broglie wavelength of 0.08 Å is achieved. Currently, this constitutes the shortest electron pulses suitable for diffraction, about sixfold shorter than in previous work. Ultrafast electron diffraction now meets the requirements for investigating the fastest primary processes in molecules and solids with atomic resolution in space and time

28-fs electron pulses for atomic-scale diffraction

Visualizing the rearrangement of atoms in a wide range of molecular and condensed-matter systems requires resolving picometer displacements on a ten-femtosecond time scale. Here we demonstrate the compression of single-electron pulses with a de Broglie wavelength of 0.08 ångström to a duration of 28±5 femtoseconds (full width at half maximum) or 12±2 femtoseconds (standard deviation), substantially shorter than any laser pulses involved. Atomic resolution diffraction from a complex organic molecule is obtained with good signalto- noise ratio within a data acquisition period of minutes. The electron-laser timing is found to be stable within 5 fs (standard deviation) over several hours, allowing pump-probe diffraction at repetitive excitation. These measurements show the feasibility of laserpump/ electron-probe scans that can resolve the fastest atomic motions relevant in reversible condensed matter transformations and organic chemistry.publishe

Interferometric time- and energy-resolved photoemission electron microscopy for few-femtosecond nanoplasmonic dynamics

We report a time-resolved normal-incidence photoemission electron microscope with an imaging time-of-flight detector using similar to 7-fs near-infrared laser pulses and a phase-stabilized interferometer for studying ultrafast nanoplasmonic dynamics via nonlinear photoemission from metallic nanostructures. The interferometer's stability (35 +/- 6 as root-mean-square from 0.2 Hz to 40 kHz) as well as on-line characterization of the driving laser field, which is a requirement for nanoplasmonic near-field reconstruction, is discussed in detail. We observed strong field enhancement and few-femtosecond localized surface plasmon lifetimes at a monolayer of self-assembled gold nanospheres with similar to 40 nm diameter and similar to 2 nm interparticle distance. A wide range of plasmon resonance frequencies could be simultaneously detected in the time domain at different nanospheres, which are distinguishable already within the first optical cycle or as close as about +/- 1 fs around time-zero. Energy-resolved imaging (microspectroscopy) additionally revealed spectral broadening due to strong-field or space charge effects. These results provide a clear path toward visualizing optically excited nanoplasmonic near-fields at ultimate spatiotemporal resolution.11Nsciescopu

Wafer-scale high-quality Ag thin film using a ZnO buffer layer for plasmonic applications

© 2020 Realizing laterally continuous, ultraflat silver (Ag) single-crystal films is a significant technological challenge. Ag thin film grown on various hetero-substrates has been used in numerous applications, due to its superior electrical and optical properties. To exploit these properties without degradation and apply these films to high-precision patterning, surface plasmonics, and so on, a high-quality thin film having an ultraflat surface and few grain boundaries is needed. A zinc oxide (ZnO) buffer layer can be used to facilitate the growth of a single-crystalline Ag thin film on a sapphire (Al2O3) substrate. ZnO films deposited on Al2O3 substrates have grain boundaries; however, Ag films grown on ZnO are nearly grain-free and close to single-crystalline quality. This can be explained by the exceptionally small extended atomic distance mismatch, of ~0.08%, between Ag and Al2O3, in which the ninth Ag atom and the eighth Al atom are matched in terms of coherence and periodicity. A modified radio frequency sputtering system with a single-crystal Ag target enabled wafer-scale growth of ultraflat, grain-free Ag films. The proposed approach using a ZnO buffer provides a new method for fabricating Ag films with high adhesion, anti-oxidative stability, and superior optical properties, and allows for easy nano-patterning11sciescopu

Large -area grain -boundary -free copper films for plasmonics

11Ysciescopu