The Free‐Electron Laser (FEL) FLASH offers the worldwide still unique capability to study ultrafast processes with high‐flux, high‐repetition rate extreme ultraviolet, and soft X‐ray pulses. The vast majority of experiments at FLASH are of pump–probe type. Many of them rely on optical ultrafast lasers. Here, a novel FEL facility laser is reported which combines high average power output from Yb:YAG amplifiers with spectral broadening in a Herriott‐type multipass cell and subsequent pulse compression to sub‐100‐fs durations. Compared to other facility lasers employing optical parametric amplification, the new system comes with significantly improved noise figures, compactness, simplicity, and power efficiency. Like FLASH, the optical laser operates with 10‐Hz burst repetition rate. The bursts consist of 800‐μs long trains of up to 800 ultrashort pulses being synchronized to the FEL with femtosecond precision. In the experimental chamber, pulses with up to 50‐μJ energy, 60‐fs full‐width half‐maximum duration and 1‐MHz rate at 1.03‐μm wavelength are available and can be adjusted by computer‐control. Moreover, nonlinear polarization rotation is implemented to improve laser pulse contrast. First cross‐correlation measurements with the FEL at the plane‐grating monochromator photon beamline are demonstrated, exhibiting the suitability of the laser for user experiments at FLASH.
The performance of time-resolved photoemission experiments at fs-pulsed photon sources is ultimately limited by the e-e Coulomb interaction, downgrading energy and momentum resolution. Here, we present an approach to effectively suppress space-charge artifacts in momentum microscopes and photoemission microscopes. A retarding electrostatic field generated by a special objective lens repels slow electrons, retaining the k-image of the fast photoelectrons. The suppression of space-charge effects scales with the ratio of the photoelectron velocities of fast and slow electrons. Fields in the range from −20 to −1100 V/mm for E kin = 100 eV to 4 keV direct secondaries and pump-induced slow electrons back to the sample surface. Ray tracing simulations reveal that this happens within the first 40 to 3 μm above the sample surface for E kin = 100 eV to 4 keV. An optimized front-lens design allows switching between the conventional accelerating and the new retarding mode. Time-resolved experiments at E kin = 107 eV using fs extreme ultraviolet probe pulses from the free-electron laser FLASH reveal that the width of the Fermi edge increases by just 30 meV at an incident pump fluence of 22 mJ/cm 2 (retarding field −21 V/mm). For an accelerating field of +2 kV/mm and a pump fluence of only 5 mJ/cm 2 , it increases by 0.5 eV (pump wavelength 1030 nm). At the given conditions, the suppression mode permits increasing the slow-electron yield by three to four orders of magnitude. The feasibility of the method at high energies is demonstrated without a pump beam at E kin = 3830 eV using hard x rays from the storage ring PETRA III. The approach opens up a previously inaccessible regime of pump fluences for photoemission experiments.
A 790-nm-driven high-harmonic generation source with a repetition rate of 6 kHz is combined with a plane-grating monochromator and a high-detection-efficiency photoelectron time-of-flight momentum microscope to enable timeand momentum-resolved photoemission spectroscopy over a spectral range of 23.6-45.5 eV with sub-100-fs time resolution. Three-dimensional (3D) Fermi surface mapping is demonstrated on graphene-covered Ir(111) with energy and momentum resolutions of 100 meV and 0.1 Å −1 , respectively. The table-top experiment sets the stage for measuring the k z -dependent ultrafast dynamics of 3D electronic structure, including band structure, Fermi surface, and carrier dynamics in 3D materials as well as 3D orbital dynamics in molecular layers.
A 790-nm-driven high-harmonic generation source with a repetition rate of 6 kHz is combined with a toroidal-grating monochromator and a high-detection-efficiency photoelectron time-of-flight momentum microscope to enable time- and momentum-resolved photoemission spectroscopy over a spectral range of 23.6–45.5 eV with sub-100 fs time resolution. Three-dimensional (3D) Fermi surface mapping is demonstrated on graphene-covered Ir(111) with energy and momentum resolutions of ≲100 meV and ≲0.1 Å−1, respectively. The tabletop experiment sets the stage for measuring the k z-dependent ultrafast dynamics of 3D electronic structure, including band structure, Fermi surface, and carrier dynamics in 3D materials as well as 3D orbital dynamics in molecular layers.
Function is dynamic and originates at atomic interfaces. Combining the degrees of freedom of molecules (1,2) with the peculiar properties of 2D quantum materials (3,4,5) can create novel functionality (6,7). Here, we report the manipulation and ultrafast imaging of a unidirectional gearing motion in molecules on a 2D quantum material. To visualize and disentangle the intertwined structural and electronic dynamics of such a hybrid interface, we record a ‘full molecular movie’ (8) by imaging the atomic positions (9,10), the evolution of the molecular orbital wavefunctions (11,12) and the modification of electronic states of the substrate (13). In a multimodal investigation in a single setup (14), we disentangle dynamics in valence and core electrons of both the molecule and the surface with femtosecond and sub-ångström precision. The ultrafast rotational motion is fueled by the transfer of hot holes into the molecules that results in “supercharging” of the film. As hot carriers move through the interface, we track a transient modification of the frontier molecular orbitals and observe a chiral symmetry breaking associated with local structural rearrangements. Our calculations show that the “supercharging” changes the interfacial potential energy landscape and triggers the gearing motion. The experiment offers all-in-one imaging of the electronic, molecular orbital, chemical and structural dynamics during the flow of charge and energy across the hybrid interface. Our approach provides detailed dynamical information on the mechanism underlying surface-adsorbed molecular gears and enables tailoring novel functionalities in hybrid active matter.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.