We demonstrate the compression of 95 keV, space-charge-dominated electron bunches to sub-100 fs durations. These bunches have sufficient charge (200 fC) and are of sufficient quality to capture a diffraction pattern with a single shot, which we demonstrate by a diffraction experiment on a polycrystalline gold foil. Compression is realized by means of velocity bunching by inverting the positive space-charge-induced velocity chirp. This inversion is induced by the oscillatory longitudinal electric field of a 3 GHz radio-frequency cavity. The arrival time jitter is measured to be 80 fs.

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RF Compression of sub-relativistic space-charge-dominated electron bunches for single-shot femtosecond electron diffraction

In this Perspective we discuss photoelectron circular dichroism (PECD), a relatively novel technique that can detect chiral molecules with high sensitivity. PECD has an enantiomeric sensitivity of typically 1–10%, which is two to three orders of magnitude larger than that of the widely employed technique of circular dichroism (CD). In PECD a chiral molecule is photoionized with circular polarized light, and the photoelectron angular scattering distribution is detected using particle imaging techniques. We present the general physical principles of photoelectron circular dichroism and we address both single- and multiphoton excitation. PECD has been measured with synchrotron radiation in single-photon ionization as well as, very recently, with femtosecond laser radiation in multiphoton ionization. We discuss the experimental implementation of PECD, focusing on velocity map coincidence imaging where the momentum distribution of both the electron and the coincident ion is measured. The coincident detection of the mass and momentum of the ion adds very powerful mass-correlated information to the PECD measurement of the chiral molecule. We illustrate the capabilities and the potential of PECD with various experimental examples and introduce computational methods that are able to model quantitatively experimental PECD results. We conclude with an outlook on novel developments and (analytical) implementations of PECD that may further broaden the application of PECD for the sensitive detection of chirality in molecules.

Detecting chirality in molecules by imaging photoelectron circular dichroism

We have developed a simple, high-speed, nearly vibration-free, mechanically scanned, optical delay line suitable for femtosecond time-resolved signal-averaging measurements. We demonstrate a 2-ps time window autocorrelator with a display updated at 400 Hz. The delay line uses a dithering planar mirror as a time-varying linear phase ramp in the spectral plane of a modified grating-lens femtosecond pulse shaper. The time delay is linearly proportional to the angular deviation of the mirror. The high speed and low vibration are a result of the extremely small angular changes required to generate a large time delay.

400-Hz mechanical scanning optical delay line

Electrons detached from atoms or molecules by photoionization carry information about the quantum state from which they originate, as well as the continuum states into which they are released. Generally, the photoelectron momentum distribution is composed of a coherent sum of angular momentum components, each with an amplitude and phase. Here we show, by using photoionization of neon, that a train of attosecond pulses synchronized with an infrared laser field can be used to disentangle these angular momentum components. Two-color, two-photon ionization via a Stark-shifted intermediate state creates an almost pure f-wave with a magnetic quantum number of zero. Interference of the f-wave with a spherically symmetric s-wave provides a holographic reference that enables phase-resolved imaging of the f-wave.

http://science.sciencemag.org/content/sci/356/6343/1150.full.pdf

Coherent imaging of an attosecond electron wave packet

UKRmol+: A suite for modelling electronic processes in molecules interacting with electrons, positrons and photons using the R-matrix method

We demonstrate the first carrier-envelope phase (CEP)-stabilized chirped pulse amplification system with pulse peak-powers in the terawatt regime. The system, which eventually is intended to be used in the generation of isolated attosecond pulses, consists of two consecutive multipass amplification stages. The first amplification stage is a commercial CEP-stable kHz system including a single 13-pass amplifier reaching a pulse energy of 2.3 mJ. Pulses are picked after the first stage at a repetition rate of 50 Hz and are further amplified in a 5-pass power-amplifier to pulse energies that reach up to 80 mJ before compression. After compression the pulse energy is 35mJ at a pulse duration of 32 fs, signifying a peak power of 1.1 terawatt. Peak-powers exceeding 1.5 TW should easily be achievable by improving the efficiency of the grating compressor. The CEP-stability of the terawatt system is demonstrated by single shot measurements of the residual CEP jitter at the full repetition rate and show an excellent root-mean-square value of 315 mrad.

Carrier-envelope phase stabilization of a terawatt level chirped pulse amplifier for generation of intense isolated attosecond pulses.

We present an experimental and theoretical investigation of the angular distributions of electrons ejected in aligned molecules by extreme ultra-violet ionization using a high harmonic generation (HHG) source. Impulsive alignment in O2, N2 and CO molecules was achieved using a near-IR laser pulse and the photoelectron angular distribution after ionization by a fs harmonic comb composed of harmonic H11 to H29 (17.5–46 eV) was recorded at the maximum of both alignment and anti-alignment. The experiment reveals signatures that are specific for the electronic orbitals that are ionized as well as the onset of the influence of the molecular structure and is well reproduced by theoretical calculations based on the multichannel Schwinger configuration interaction method.

Photoelectron kinetic and angular distributions for the ionization of aligned molecules using a HHG source

The use of a new type in-vacuum pixel detector in velocity map imaging (VMI) is introduced The Medipix2 and Timepix semiconductor pixel detectors (256×256 square pixels, 55×55 μm2) are well suited for charged particle detection They offer high resolution, low noise, and high quantum efficiency The Medipix2 chip allows double energy discrimination by offering a low and a high energy threshold The Timepix detector allows to record the incidence time of a particle with a temporal resolution of 10 ns and a dynamic range of 160 μs Results of the first time application of the Medipix2 detector to VMI are presented, investigating the quantum efficiency as well as the possibility to operate at increased background pressure in the vacuum chamber

Velocity map imaging using an in-vacuum pixel detector

We present measurements of photoelectron angular distributions (PADs) for the ionization of aligned CO2 molecules by an extreme ultraviolet laser pulse (17–45 eV) that is produced via high-harmonic generation, and that is polarized perpendicularly to the alignment laser axis. Differential PADs are recorded by taking the difference between two measurements for aligned and anti-aligned molecules. The results are compared with ab initio multi-channel R-matrix calculations, which are extended to include the computation of PADs. The calculations agree very well with the experiment, and are resolved with respect to the internal state of the ion and the polarization of the ionizing laser field relative to the molecular frame. For a sufficiently high, but experimentally achievable degree of alignment, the nodal structure of the molecular orbital becomes visible in the PAD.

https://iopscience.iop.org/article/10.1088/0953-4075/47/12/124017/pdf

Georg Gademann

Papers

Carrier-envelope phase stabilization of a terawatt level chirped pulse amplifier for generation of intense isolated attosecond pulses.

Photoelectron kinetic and angular distributions for the ionization of aligned molecules using a HHG source

Velocity map imaging using an in-vacuum pixel detector

Imaging the electronic structure of valence orbitals in the XUV ionization of aligned molecules

Expanding the attosecond toolbox: demonstration of novel experiments, new light sources and detectors