We present the first demonstration of THz driven bunch compression and timing stabilization of a relativistic electron beam. Quasi-single-cycle strong field THz radiation is used in a shorted ...parallel-plate structure to compress a few-fC beam with 2.5 MeV kinetic energy by a factor of 2.7, producing a 39 fs rms bunch length and a reduction in timing jitter by more than a factor of 2 to 31 fs rms. This THz driven technique offers a significant improvement to beam performance for applications like ultrafast electron diffraction, providing a critical step towards unprecedented timing resolution in ultrafast sciences, and other accelerator applications using femtosecond-scale electron beams.
The ultrafast photoinduced ring-opening of 1,3-cyclohexadiene constitutes a textbook example of electrocyclic reactions in organic chemistry and a model for photobiological reactions in vitamin D ...synthesis. Although the relaxation from the photoexcited electronic state during the ring-opening has been investigated in numerous studies, the accompanying changes in atomic distance have not been resolved. Here we present a direct and unambiguous observation of the ring-opening reaction path on the femtosecond timescale and subångström length scale using megaelectronvolt ultrafast electron diffraction. We followed the carbon-carbon bond dissociation and the structural opening of the 1,3-cyclohexadiene ring by the direct measurement of time-dependent changes in the distribution of interatomic distances. We observed a substantial acceleration of the ring-opening motion after internal conversion to the ground state due to a steepening of the electronic potential gradient towards the product minima. The ring-opening motion transforms into rotation of the terminal ethylene groups in the photoproduct 1,3,5-hexatriene on the subpicosecond timescale.
We demonstrate single-shot temporal characterization of relativistic electron bunches using single-cycle terahertz (THz) field streaking. A transverse deflecting structure consisting of a metal slit ...enables efficient coupling of the THz field and electron bunch. The intrinsically stable carrier envelope phase and strong gradient of the THz pulses allow simultaneous, self-calibrated determination of the time-of-arrival with subfemtosecond precision and bunch duration with single-femtosecond precision, respectively, opening up new opportunities for ultrafast electron diffraction as well as accelerator technologies in general.
•We experimentally demonstrated a time-resolved electron microdiffraction technique using mega-electron-volt electrons for studies of ultrafast structural dynamics over localized crystalline ...domains•The high resolving power of this technique with 5 um (root mean square) electron probe size was demonstrated by high SNR diffraction pattern from a 10 um paraffin crystal.•The high temporal resolution of this technique was estimated to be 100 fs (root mean square) from the time-resolved phonon softening mode in optical-pumped polycrystalline Bi.•This technique delivers pulses of 10k electrons at 4.2 MeV energy with a normalized emittance of 3 nm-rad at 180 Hz repetition rate.•This new characterization capability will open many research opportunities in material and biological sciences.
To understand and control the basic functions of physical, chemical and biological processes from micron to nano-meter scale, an instrument capable of visualizing transient structural changes of inhomogeneous materials with atomic spatial and temporal resolutions, is required. One such technique is femtosecond electron microdiffraction, in which a short electron pulse with femtosecond-scale duration is focused into a micron-scale spot and used to obtain diffraction images to resolve ultrafast structural dynamics over a localized crystalline domain. In this letter, we report the experimental demonstration of time-resolved mega-electron-volt electron microdiffraction which achieves a 5 μm root-mean-square (rms) beam size on the sample and a 110 fs rms temporal resolution. Using pulses of 10k electrons at 4.2 MeV energy with a normalized emittance 3 nm-rad, we obtained high quality diffraction from a single 10 μm paraffin (C44H90) crystal. The phonon softening mode in optical-pumped polycrystalline Bi was also time-resolved, demonstrating the temporal resolution limits of the instrument. This new characterization capability will open many research opportunities in material and biological sciences.
The radiolysis of water is ubiquitous in nature and plays a critical role in numerous biochemical and technological applications. Although the elementary reaction pathways for ionized water have been ...studied, the short-lived intermediate complex and structural dynamic response after the proton transfer reaction remain poorly understood. Using a liquid-phase ultrafast electron diffraction technique to measure the intermolecular oxygen···oxygen and oxygen···hydrogen bonds, we captured the short-lived radical-cation complex OH(H
O
) that was formed within 140 femtoseconds through a direct oxygen···oxygen bond contraction and proton transfer, followed by the radical-cation pair dissociation and the subsequent structural relaxation of water within 250 femtoseconds. These measurements provide direct evidence of capturing this metastable radical-cation complex before separation, thereby improving our fundamental understanding of elementary reaction dynamics in ionized liquid water.
Echo-enabled harmonic generation free electron lasers hold great promise for the generation of fully coherent radiation in x-ray wavelengths. Here we report the first evidence of high harmonics from ...the echo-enabled harmonic generation technique in the realistic scenario where the laser energy modulation is comparable to the beam slice energy spread. In this experiment, coherent radiation at the seventh harmonic of the second seed laser is generated when the energy modulation amplitude is about 2-3 times the slice energy spread. The experiment confirms the underlying physics of echo-enabled harmonic generation and may have a strong impact on emerging seeded x-ray free electron lasers that are capable of generating laserlike x rays which will advance many areas of science.
The photo-induced dynamics of
-nitrophenol, particularly its photolysis, has garnered significant scientific interest as a potential source of nitrous acid in the atmosphere. Although the photolysis ...products and preceding photo-induced electronic structure dynamics have been investigated extensively, the nuclear dynamics accompanying the non-radiative relaxation of
-nitrophenol on the ultrafast timescale, which include an intramolecular proton transfer step, have not been experimentally resolved. Herein, we present a direct observation of the ultrafast nuclear motions mediating photo-relaxation using ultrafast electron diffraction. This work spatiotemporally resolves the loss of planarity which enables access to a conical intersection between the first excited state and the ground state after the proton transfer step, on the femtosecond timescale and with sub-Angstrom resolution. Our observations, supported by
multiple spawning simulations, provide new insights into the proton transfer mediated relaxation mechanism in
-nitrophenol.
We report the first experimental demonstration of the echo-enabled harmonic generation technique, which holds great promise for generation of high-power, fully coherent short-wavelength radiation. In ...this experiment, coherent radiation at the 3rd and 4th harmonics of the second seed laser is generated from the so-called beam echo effect. The experiment confirms the physics behind this technique and paves the way for applying the echo-enabled harmonic generation technique for seeded x-ray free electron lasers.
Monomers and dimers of spherical gold nanoparticles (NPs) exhibit highly uniform plasmonic properties at the single-particle level due to their high structural homogeneity (precision plasmonics). ...Recent investigations in precision plasmonics have largely focused on static properties using conventional techniques such as transmission electron microscopy and optical dark-field microscopy. In this Feature Article, we first highlight the application of femtosecond time-resolved electron diffraction for monitoring the nonequilibrium dynamics of spherical gold NPs after ultrafast optical excitation. The analysis of the transient diffraction patterns allows us to directly obtain quantitative information on the incoherent excitation of the lattice, that is, heating upon electron–lattice equilibration, as well as on the development of strain due to lattice expansion on picosecond time scales. The controlled assembly of two spherical gold NPs into a dimer with a few nanometers gap leads to unique optical properties. Specifically, extremely high electric fields (hot spot) in the gap are generated upon resonant optical excitation. Conventional optical microscopy cannot spatially resolve this unique hot spot due to the optical diffraction limit. We therefore employed nonlinear photoemission electron microscopy to visualize hot spots in single dimers of spherical gold NPs. A quantitative comparison of different single dimers confirms the homogeneity of the hot spots on the single-particle level. Overall, these initial results are highly encouraging because they pave the way to investigate nonequilibrium dynamics in highly uniform plasmonic nanostructures at the time and space limits.
PDF
