Sizes of pure and doped helium droplets from single shot x-ray imaging.

Advancements in x-ray free-electron lasers on producing ultrashort, ultrabright, and coherent x-ray pulses enable single-shot imaging of fragile nanostructures, such as superfluid helium droplets. This imaging technique gives unique access to the sizes and shapes of individual droplets. In the past, such droplet characteristics have only been indirectly inferred by ensemble averaging techniques. Here, we report on the size distributions of both pure and doped droplets collected from single-shot x-ray imaging and produced from the free-jet expansion of helium through a 5 µm diameter nozzle at 20 bars and nozzle temperatures ranging from 4.2 to 9 K. This work extends the measurement of large helium nanodroplets containing 109-1011 atoms, which are shown to follow an exponential size distribution. Additionally, we demonstrate that the size distributions of the doped droplets follow those of the pure droplets at the same stagnation condition but with smaller average sizes.

Communication: X-ray coherent diffractive imaging by immersion in nanodroplets.

Lensless x-ray microscopy requires the recovery of the phase of the radiation scattered from a specimen. Here, we demonstrate a de novo phase retrieval technique by encapsulating an object in a superfluid helium nanodroplet, which provides both a physical support and an approximate scattering phase for the iterative image reconstruction. The technique is robust, fast-converging, and yields the complex density of the immersed object. Images of xenon clusters embedded in superfluid helium droplets reveal transient configurations of quantum vortices in this fragile system.

Sub-nanosecond time-resolved ambient-pressure X-ray photoelectron spectroscopy setup for pulsed and constant wave X-ray light sources.

An apparatus for sub-nanosecond time-resolved ambient-pressure X-ray photoelectron spectroscopy studies with pulsed and constant wave X-ray light sources is presented. A differentially pumped hemispherical electron analyzer is equipped with a delay-line detector that simultaneously records the position and arrival time of every single electron at the exit aperture of the hemisphere with ~0.1 mm spatial resolution and ~150 ps temporal accuracy. The kinetic energies of the photoelectrons are encoded in the hit positions along the dispersive axis of the two-dimensional detector. Pump-probe time-delays are provided by the electron arrival times relative to the pump pulse timing. An average time-resolution of (780 ± 20) ps (FWHM) is demonstrated for a hemisphere pass energy E(p) = 150 eV and an electron kinetic energy range KE = 503-508 eV. The time-resolution of the setup is limited by the electron time-of-flight (TOF) spread related to the electron trajectory distribution within the analyzer hemisphere and within the electrostatic lens system that images the interaction volume onto the hemisphere entrance slit. The TOF spread for electrons with KE = 430 eV varies between ~9 ns at a pass energy of 50 eV and ~1 ns at pass energies between 200 eV and 400 eV. The correlation between the retarding ratio and the TOF spread is evaluated by means of both analytical descriptions of the electron trajectories within the analyzer hemisphere and computer simulations of the entire trajectories including the electrostatic lens system. In agreement with previous studies, we find that the by far dominant contribution to the TOF spread is acquired within the hemisphere. However, both experiment and computer simulations show that the lens system indirectly affects the time resolution of the setup to a significant extent by inducing a strong dependence of the angular spread of electron trajectories entering the hemisphere on the retarding ratio. The scaling of the angular spread with the retarding ratio can be well approximated by applying Liouville's theorem of constant emittance to the electron trajectories inside the lens system. The performance of the setup is demonstrated by characterizing the laser fluence-dependent transient surface photovoltage response of a laser-excited Si(100) sample.

Helium superfluidity. Shapes and vorticities of superfluid helium nanodroplets.

Helium nanodroplets are considered ideal model systems to explore quantum hydrodynamics in self-contained, isolated superfluids. However, exploring the dynamic properties of individual droplets is experimentally challenging. In this work, we used single-shot femtosecond x-ray coherent diffractive imaging to investigate the rotation of single, isolated superfluid helium-4 droplets containing ~10(8) to 10(11) atoms. The formation of quantum vortex lattices inside the droplets is confirmed by observing characteristic Bragg patterns from xenon clusters trapped in the vortex cores. The vortex densities are up to five orders of magnitude larger than those observed in bulk liquid helium. The droplets exhibit large centrifugal deformations but retain axially symmetric shapes at angular velocities well beyond the stability range of viscous classical droplets.

Atomic-Scale Perspective of Ultrafast Charge Transfer at a Dye-Semiconductor Interface.

Understanding interfacial charge-transfer processes on the atomic level is crucial to support the rational design of energy-challenge relevant systems such as solar cells, batteries, and photocatalysts. A femtosecond time-resolved core-level photoelectron spectroscopy study is performed that probes the electronic structure of the interface between ruthenium-based N3 dye molecules and ZnO nanocrystals within the first picosecond after photoexcitation and from the unique perspective of the Ru reporter atom at the center of the dye. A transient chemical shift of the Ru 3d inner-shell photolines by (2.3 ± 0.2) eV to higher binding energies is observed 500 fs after photoexcitation of the dye. The experimental results are interpreted with the aid of ab initio calculations using constrained density functional theory. Strong indications for the formation of an interfacial charge-transfer state are presented, providing direct insight into a transient electronic configuration that may limit the efficiency of photoinduced free charge-carrier generation.

Differential near-edge coherent diffractive imaging using a femtosecond high-harmonic XUV light source.

Element-specific contrast enhancement in tabletop coherent diffractive imaging (CDI) is demonstrated by employing an ultrafast extreme ultraviolet (XUV) light source with tunable photon energy. By combining two measurements performed at energies below and above the Al L(2,3) absorption edge, the spatial autocorrelation function of a micron-scale double pinhole in a 300 nm thick aluminum foil is retrieved despite a dominant background signal from directly transmitted light across the entire range of detectable diffraction angles. The fringe visibility in the diffraction patterns is 0 below the Al L(2,3) edge, 0.53 ± 0.06 above the edge, and 0.73 ± 0.08 in the differential image that combines the two measurements. The proof-of-principle experiment demonstrates that the variations of XUV optical constants in the vicinity of an inner-shell absorption edge can be utilized to improve the chemical sensitivity and image reconstruction quality of laboratory-based ultrafast imaging experiments.

Parametrically polarization shaped pulses guided via a hollow core photonic crystal fiber for coherent control.

We present ultrafast polarization pulse shaping through a micro structured hollow core photonic crystal fiber. The pulses are shaped in pulse sequences in which the energy, distance, phases, and chirps as well as the state of polarization of each individual sub-pulse can be independently controlled. The application of these pulses for coherent control is demonstrated for feedback loop optimization of the multi-photon ionization of potassium dimers. In a second experiment, this process is investigated by shaper-assisted pump-probe spectroscopy which is likewise performed with pulses that are transmitted through the fiber. Both techniques reveal the excitation pathway including the dynamics in the participating electronic states and expose the relevance of the polarization. These methods will be valuable for endoscopic applications.

Reconstruction of polarization-shaped laser pulses after a hollow-core fiber using backreflection.

We present a method to reconstruct the pulse shape of polarization-shaped femtosecond laser pulses after a hollow-core photonic crystal fiber by reflecting the pulses back through the fiber. First, a procedure is introduced to receive the optical fiber properties and generate parametrically shaped pulses after propagation through the fiber. Changes of the fiber's birefringence by mechanical stress are examined to investigate the correlation between the pulse shapes after one and two passes through the fiber. Finally, we demonstrate the characterization of the pulse after one pass through the fiber by calculating the pulse shape from the measured pulse after two passes.

Full control over the electric field using four liquid crystal arrays.

We present a femtosecond pulse shaper setup that is capable of shaping the phase, amplitude, and polarization simultaneously and independently. The modulator utilizes four liquid crystal arrays, a pair of half-wave plates, and a polarizer to gain full control of the electrical field. This is done in a common-path common-optic scheme without using interferometry. The functionality of the setup is demonstrated by using systematic parameter scans and example pulses.

Parametric polarization pulse shaping demonstrated for optimal control of NaK.

We present a routine for calculating and producing customized/parametric femtosecond laser pulses for investigating molecular processes involving the polarization. It is applied on the ionization of NaK molecules by feedback-loop optimization using the recently introduced double-pass "serial setup" that is capable of phase, amplitude, and polarization modulation. The temporal subpulse encoding uses the parameters distance, intensity, zero order spectral phase, and polarization state.

Interferometric generation of parametrically shaped polarization pulses.

We demonstrate the capabilities of the recently introduced interferometric parallel pulse shaper setup and present a method for fully tailoring the three-dimensional electrical field of femtosecond laser pulses. The possibility of producing parametric polarization pulses with arbitrary orientations and ellipticities in time is demonstrated with a selection of example pulses.

Phase, amplitude, and polarization shaping with a pulse shaper in a Mach-Zehnder interferometer.

We present a shaper scheme that fully controls the spectral phase, amplitude, and polarization of femtosecond laser pulses. In particular, it enables independent manipulation over the major axis orientation and the axis ratio of the polarization ellipse. This is accomplished by integrating a 4f-shaper setup in both arms of a Mach-Zehnder interferometer and rotating the polarization by 90 degrees in one of the arms before overlaying the beams. The generated pulses are resolved in a simple and intuitive detection scheme.