Allan S. Johnson

Spatio-temporal characterization of intense few-cycle 2 μm pulses

We present a variant of spatially encoded spectral shearing interferometry for measuring two-dimensional spatio-temporal slices of few-cycle pulses centered around 2 μm. We demonstrate experimentally that the device accurately retrieves the pulse-front tilt caused by angular dispersion of two-cycle pulses. We then use the technique to characterize 500-650 μJ pulses from a hollow fiber pulse compressor, with durations as short as 7.1 fs (1.3 optical cycles).

Practical witness for electronic coherences

The origin of the coherences in two-dimensional spectroscopy of photosynthetic complexes remains disputed. Recently, it has been shown that in the ultrashort-pulse limit, oscillations in a frequency-integrated pump-probe signal correspond exclusively to electronic coherences, and thus such experiments can be used to form a test for electronic vs. vibrational oscillations in such systems. Here, we demonstrate a method for practically implementing such a test, whereby pump-probe signals are taken at several different pulse durations and used to extrapolate to the ultrashort-pulse limit. We present analytic and numerical results determining requirements for pulse durations and the optimal choice of pulse central frequency, which can be determined from an absorption spectrum. Our results suggest that for numerous systems, the required experiment could be implemented by many ultrafast spectroscopy laboratories using pulses of tens of femtoseconds in duration. Such experiments could resolve the standing debate over the nature of coherences in photosynthetic complexes.

High-flux soft x-ray harmonic generation from ionization-shaped few-cycle laser pulses

X-ray harmonics made with long-wavelength lasers reach higher fluxes and photon energies when plasma effects dominate. Laser-driven high-harmonic generation provides the only demonstrated route to generating stable, tabletop attosecond x-ray pulses but has low flux compared to other x-ray technologies. We show that high-harmonic generation can produce higher photon energies and flux by using higher laser intensities than are typical, strongly ionizing the medium and creating plasma that reshapes the driving laser field. We obtain high harmonics capable of supporting attosecond pulses up to photon energies of 600 eV and a photon flux inside the water window (284 to 540 eV) 10 times higher than previous attosecond sources. We demonstrate that operating in this regime is key for attosecond pulse generation in the x-ray range and will become increasingly important as harmonic generation moves to even longer-wavelength driving fields.

Accurate prediction of X-ray pulse properties from a free-electron laser using machine learning

A. Sanchez-Gonzalez,1 P. Micaelli,1 C. Olivier,1 T. R. Barillot,1 M. Ilchen,2, 3 A. A. Lutman,4 A. Marinelli,4 T. Maxwell,4 A. Achner,3 M. Agåker,5 N. Berrah,6 C. Bostedt,4, 7 J. Buck,8 P. H. Bucksbaum,2, 9 S. Carron Montero,4, 10 B. Cooper,1 J. P. Cryan,2 M. Dong,5 R. Feifel,11 L. J. Frasinski,1 H. Fukuzawa,12 A. Galler,3 G. Hartmann,8, 13 N. Hartmann,4 W. Helml,4, 14 A. S. Johnson,1 A. Knie,13 A. O. Lindahl,2, 11 J. Liu,3 K. Motomura,12 M. Mucke,5 C. O’Grady,4 J-E. Rubensson,5 E. R. Simpson,1 R. J. Squibb,11 C. Såthe,15 K. Ueda,12 M. Vacher,16, 17 D. J. Walke,1 V. Zhaunerchyk,11 R. N. Coffee,4 and J. P. Marangos1 1Department of Physics, Imperial College, London, SW7 2AZ, United Kingdom 2Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA 3European XFEL GmbH, Holzkoppel 4, 22869 Schenefeld, Germany 4Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA 5Department of Physics and Astronomy, Uppsala University, Uppsala, 75120, Sweden 6Department of Physics, University of Connecticut, 2152 Hillside Road, U-3046, Storrs, CT 06269, USA 7Argonne National Laboratory, Lemont, IL 60439, USA 8Deutsches Elektronen-Synchrotron DESY, Notkestrasse 85, Hamburg, 22607, Germany 9Department of Physics, Stanford University, 382 Via Pueblo Mall, Stanford, CA 94305, USA 10California Lutheran University, 60 W Olsen Rd, Thousand Oaks, CA 91360, USA 11Department of Physics, University of Gothenburg, Origovägen 6B, 41296 Gothenburg, Sweden 12Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577, Japan 13Institut für Physik und CINSaT, Universität Kassel, Heinrich-Plett-Str. 40, 34132 Kassel, Germany 14Physics Department, TU Munich, James-Franck-Str. 1, 85748 Garching, Germany 15MAX IV Laboratory, Lund University, Box 118, SE-221 00 Lund, Sweden 16Department of Chemistry, Imperial College London, London SW7 2AZ, United Kingdom 17Department of Chemistry Ångtröm, Uppsala University, Uppsala, 75120, SwedenFree-electron lasers providing ultra-short high-brightness pulses of X-ray radiation have great potential for a wide impact on science, and are a critical element for unravelling the structural dynamics of matter. To fully harness this potential, we must accurately know the X-ray properties: intensity, spectrum and temporal profile. Owing to the inherent fluctuations in free-electron lasers, this mandates a full characterization of the properties for each and every pulse. While diagnostics of these properties exist, they are often invasive and many cannot operate at a high-repetition rate. Here, we present a technique for circumventing this limitation. Employing a machine learning strategy, we can accurately predict X-ray properties for every shot using only parameters that are easily recorded at high-repetition rate, by training a model on a small set of fully diagnosed pulses. This opens the door to fully realizing the promise of next-generation high-repetition rate X-ray lasers.

An apparatus for quantitative high-harmonic generation spectroscopy in molecular vapours

We present an apparatus for performing gas phase high-harmonic generation spectroscopy of molecules primarily found in the liquid phase. Liquid molecular samples are heated in a temperature controlled bath and their vapour is used to back a continuous flow gas jet, with vapour pressures of over 1 bar possible. In order to demonstrate the system, we perform high harmonic spectroscopy experiments in benzene with a 1.8 μm driving field. Using the unique capabilities of the system, we obtain spectra that are nearly free from the effects of longitudinal phase-matching, amenable to comparison with advanced numerical modelling.

Coincidence timing of femtosecond optical pulses in an X-ray free electron laser

Femtosecond resolution pump-probe experiments are now routinely carried out at X-ray Free Electron Lasers, enabled by the development of cross-correlation “time-tools” which correct the picosecond-level jitter between the optical and X-ray pulses. These tools provide very accurate, <10 fs, measurement of the relative arrival time, but do not provide a measure of the absolute coincidence time in the interaction. Cross-correlation experiments using transient reflectivity in a crystal are commonly used for this purpose, and to date no quantitative analysis of the accuracy or stability of absolute coincidence time determination has been performed. We have performed a quantitative analysis of coincidence timing at the SACLA facility through a cross-correlation of 100 ± 10 fs, 400 nm optical pulses with 7 fs, 10.5 keV X-ray pulses via transient reflectivity in a cerium-doped yttrium aluminum garnet crystal. We have modelled and fit the transient reflectivity, which required a convolution with a 226 ± 12 fs unce...

X-ray Free Electron Laser Determination of Crystal Structures of Dark and Light States of a Reversibly Photoswitching Fluorescent Protein at Room Temperature.

The photochromic fluorescent protein Skylan-NS (Nonlinear Structured illumination variant mEos3.1H62L) is a reversibly photoswitchable fluorescent protein which has an unilluminated/ground state with an anionic and cis chromophore conformation and high fluorescence quantum yield. Photo-conversion with illumination at 515 nm generates a meta-stable intermediate with neutral trans-chromophore structure that has a 4 h lifetime. We present X-ray crystal structures of the cis (on) state at 1.9 Angstrom resolution and the trans (off) state at a limiting resolution of 1.55 Angstrom from serial femtosecond crystallography experiments conducted at SPring-8 Angstrom Compact Free Electron Laser (SACLA) at 7.0 keV and 10.5 keV, and at Linac Coherent Light Source (LCLS) at 9.5 keV. We present a comparison of the data reduction and structure determination statistics for the two facilities which differ in flux, beam characteristics and detector technologies. Furthermore, a comparison of droplet on demand, grease injection and Gas Dynamic Virtual Nozzle (GDVN) injection shows no significant differences in limiting resolution. The photoconversion of the on- to the off-state includes both internal and surface exposed protein structural changes, occurring in regions that lack crystal contacts in the orthorhombic crystal form.

Femtosecond Laser Mass Spectrometry and High Harmonic Spectroscopy of Xylene Isomers

Structural isomers, molecules having the same chemical formula but with atoms bonded in different order, are hard to identify using conventional spectroscopy and mass spectrometry. They exhibit virtually indistinguishable mass spectra when ionized by electrons. Laser mass spectrometry based on photoionization of the isomers has emerged as a promising alternative but requires shaped ultrafast laser pulses. Here we use transform limited femtosecond pulses to distinguish the isomers using two methods. First, we probe doubly charged parent ions with circularly polarized light. We show that the yield of doubly charged ortho-xylene decreases while para-xylene increases over a range of laser intensities when the laser polarization is changed from linear to circular. Second, we probe high harmonic generation from randomly oriented isomer molecules subjected to an intense laser field. We show that the yield of high-order harmonics varies with the positioning of the methyl group in xylene isomers (ortho-, para- and meta-) and is due to differences in the strength of tunnel ionization and the overlap between the angular peaks of ionization and photo-recombination.

Author Correction: Femtosecond Laser Mass Spectrometry and High Harmonic Spectroscopy of Xylene Isomers

A correction to this article has been published and is linked from the HTML and PDF versions of this paper. The error has been fixed in the paper.

Apparatus for soft x-ray table-top high harmonic generation

There has been considerable recent interest in tabletop soft X-ray attosecond sources enabled by the new generation of intense, few-cycle laser sources at operating wavelengths longer than 800 nm. In our recent work [Johnson et al., Sci. Adv. 4(5), eaar3761 (2018)], we have demonstrated a new regime for the generation of X-ray attosecond pulses in the water window (284-540 eV) by high-harmonic generation, which resulted in soft X-ray fluxes of ≈109 photons/s and a maximum photon energy of 600 eV, an order of magnitude and 50 eV higher, respectively, than previously attained with few-cycle drivers. Here we present the key elements of our apparatus for the generation and detection of soft X-ray high harmonic radiation in the water window. Of critical importance is a differentially pumped gas target capable of supporting the multi-atmospheric pressures required to phase-match the high energy emission while strongly constraining the gas density, suppressing the effects of ionization and absorption outside the interaction region.