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View article: Attosecond X-Ray Core-Level Chronoscopy of Aromatic Molecules
Attosecond X-Ray Core-Level Chronoscopy of Aromatic Molecules Open
Attosecond photoemission or photoionization delays are a unique probe of the structure and the electronic dynamics of matter. However, the spectral congestion of valence photoelectron spectra sets fundamental limits to the complexity of sy…
View article: Imaging Valence Electron Rearrangement in a Chemical Reaction Using Hard X-Ray Scattering
Imaging Valence Electron Rearrangement in a Chemical Reaction Using Hard X-Ray Scattering Open
We have observed the signatures of valence electron rearrangement in photoexcited ammonia using ultrafast hard x-ray scattering. Time-resolved x-ray scattering is a powerful tool for imaging structural dynamics in molecules because of the …
View article: The time-resolved atomic, molecular and optical science instrument at the Linac Coherent Light Source. Corrigendum
The time-resolved atomic, molecular and optical science instrument at the Linac Coherent Light Source. Corrigendum Open
The name of an author in the article by Walter et al. (2022) [ J. Synchrotron Rad. 29 , 957–968] is corrected.
View article: Nonlinear reversal of photo-excitation on the attosecond time scale improves ultrafast x-ray diffraction images
Nonlinear reversal of photo-excitation on the attosecond time scale improves ultrafast x-ray diffraction images Open
The advent of isolated and intense sub-femtosecond X-ray pulses enables tracking of quantummechanical motion of electrons in molecules and solids. The combination of X-ray spectroscopy and diffraction imaging is a powerful approach to visu…
View article: Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites
Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites Open
The detailed understanding of electronic coherence in quantum systems requires measurements on the attosecond timescale. Attosecond x-ray pulses enable the study of electronic coherence in core-excited molecular systems. Here we report on …
View article: Design and performance of a magnetic bottle electron spectrometer for high-energy photoelectron spectroscopy
Design and performance of a magnetic bottle electron spectrometer for high-energy photoelectron spectroscopy Open
We describe the design and performance of a magnetic bottle electron spectrometer (MBES) for high-energy electron spectroscopy. Our design features a 2 m long electron drift tube and electrostatic retardation lens, achieving sub-electronvo…
View article: Covariance Analysis of Impulsive Streaking
Covariance Analysis of Impulsive Streaking Open
We present a comprehensive framework of modeling covariance in angular streaking experiments. Within the impulsive streaking regime, the displacement of electron momentum distribution (MD) provides a tight connection between the dressing-f…
View article: “Beam à la carte”: Laser heater shaping for attosecond pulses in a multiplexed x-ray free-electron laser
“Beam à la carte”: Laser heater shaping for attosecond pulses in a multiplexed x-ray free-electron laser Open
Electron beam shaping allows the control of the temporal properties of x-ray free-electron laser pulses from femtosecond to attosecond timescales. Here, we demonstrate the use of a laser heater to shape electron bunches and enable the gene…
View article: Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule
Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule Open
In molecular systems, the ultrafast motion of electrons initiates the process of chemical change. Tracking this electronic motion across molecules requires coupling attosecond time resolution to atomic-scale spatial sensitivity. In this wo…
View article: Attosecond impulsive stimulated X-ray Raman scattering in liquid water
Attosecond impulsive stimulated X-ray Raman scattering in liquid water Open
We report the measurement of impulsive stimulated x-ray Raman scattering in neutral liquid water. An attosecond pulse drives the excitations of an electronic wavepacket in water molecules. The process comprises two steps: a transition to c…
View article: Fragment correlation mass spectrometry: Determining the structures of biopolymers in a complex mixture without isolating individual components
Fragment correlation mass spectrometry: Determining the structures of biopolymers in a complex mixture without isolating individual components Open
Fragment correlation mass spectrometry correlates ion pairs generated from the same fragmentation pathway, achieved by covariance mapping of tandem mass spectra generated with an unmodified linear ion trap without preseparation. We enable …
View article: Fragment correlation mass spectrometry enables direct characterization of di-sulfide cleavage pathways of therapeutic peptides
Fragment correlation mass spectrometry enables direct characterization of di-sulfide cleavage pathways of therapeutic peptides Open
Therapeutic peptides that are connected by disulfide bonds are often difficult to analyze by traditional tandem mass spec-trometry without chemical modification. Using fragment correlation mass spectrometry, we measured 56 pairs of fragmen…
View article: Fragment correlation mass spectrometry: determining the structures of biopolymers in a complex mixture without isolating individual components
Fragment correlation mass spectrometry: determining the structures of biopolymers in a complex mixture without isolating individual components Open
Fragment correlation mass spectrometry correlates ion pairs generated from the same fragmentation pathway, achieved by covariance mapping of tandem mass spectra generated with an unmodified linear ion trap without pre-separation. We enable…
View article: The Role of Momentum Partitioning in Covariance Ion Imaging Analysis
The Role of Momentum Partitioning in Covariance Ion Imaging Analysis Open
We present results from a covariance ion imaging study, which employs extensive filtering, on the relationship between fragment momenta to gain deeper insight into photofragmentation dynamics. A new data analysis approach is introduced tha…
View article: "Beam `a la carte": laser heater shaping for attosecond pulses in a multiplexed x-ray free-electron laser
"Beam `a la carte": laser heater shaping for attosecond pulses in a multiplexed x-ray free-electron laser Open
Electron beam shaping allows the control of the temporal properties of x-ray free-electron laser pulses from femtosecond to attosecond timescales. Here we demonstrate the use of a laser heater to shape electron bunches and enable the gener…
View article: Spectrotemporal shaping of attosecond x-ray pulses with a fresh-slice free-electron laser
Spectrotemporal shaping of attosecond x-ray pulses with a fresh-slice free-electron laser Open
We propose a scheme allowing coherent shaping, i.e., controlling both the amplitude and phase, of attosecond x-ray pulses at free-electron lasers. We show that by seeding an FEL with a short coherent seed that overfills the amplification b…
View article: Attosecond X-ray Core-level Chronoscopy of Aromatic Molecules
Attosecond X-ray Core-level Chronoscopy of Aromatic Molecules Open
Attosecond photoemission or photoionization delays are a unique probe of the structure and the electronic dynamics of matter. However, spectral congestion and spatial delocalization of valence electron wave functions set fundamental limits…
View article: Attosecond Delays in X-ray Molecular Ionization
Attosecond Delays in X-ray Molecular Ionization Open
The photoelectric effect is not truly instantaneous, but exhibits attosecond delays that can reveal complex molecular dynamics. Sub-femtosecond duration light pulses provide the requisite tools to resolve the dynamics of photoionization. A…
View article: Experimental Demonstration of Attosecond Pump-Probe Spectroscopy with an X-ray Free-Electron Laser
Experimental Demonstration of Attosecond Pump-Probe Spectroscopy with an X-ray Free-Electron Laser Open
Pump-probe experiments with sub-femtosecond resolution are the key to understanding electronic dynamics in quantum systems. Here we demonstrate the generation and control of sub-femtosecond pulse pairs from a two-colour X-ray free-electron…
View article: Efficient prediction of attosecond two-colour pulses from an X-ray free-electron laser with machine learning
Efficient prediction of attosecond two-colour pulses from an X-ray free-electron laser with machine learning Open
X-ray free-electron lasers are sources of coherent, high-intensity X-rays with numerous applications in ultra-fast measurements and dynamic structural imaging. Due to the stochastic nature of the self-amplified spontaneous emission process…
View article: Direct momentum imaging of charge transfer following site-selective ionization
Direct momentum imaging of charge transfer following site-selective ionization Open
We study ultrafast charge rearrangement in dissociating 2-iodopropane (2-C3H7I) using site-selective core-ionization at the iodine atom. Clear signatures of electron transfer between the neutral propyl fragment and multiply charged iodine …
View article: Compact single-shot soft X-ray photon spectrometer for free-electron laser diagnostics
Compact single-shot soft X-ray photon spectrometer for free-electron laser diagnostics Open
The photon spectrum from free-electron laser (FEL) light sources offers valuable information in time-resolved experiments and machine optimization in the spectral and temporal domains. We have developed a compact single-shot photon spectro…
View article: Time-Resolved X-ray Photoelectron Spectroscopy: Ultrafast Dynamics in CS<sub>2</sub>Probed at the S 2p Edge
Time-Resolved X-ray Photoelectron Spectroscopy: Ultrafast Dynamics in CS<sub>2</sub>Probed at the S 2p Edge Open
Recent developments in X-ray free-electron lasers have enabled a novel site-selective probe of coupled nuclear and electronic dynamics in photoexcited molecules, time-resolved X-ray photoelectron spectroscopy (TRXPS). We present results fr…
View article: Streaking single-electron ionization in open-shell molecules driven by x-ray pulses
Streaking single-electron ionization in open-shell molecules driven by x-ray pulses Open
We obtain continuum molecular wavefunctions for open-shell molecules in the Hartree-Fock framework. We do so while accounting for the singlet or triplet total spin symmetry of the molecular ion, that is, of the open-shell orbital and the i…
View article: Identification of Cofragmented Combinatorial Peptide Isomers by Two-Dimensional Partial Covariance Mass Spectrometry
Identification of Cofragmented Combinatorial Peptide Isomers by Two-Dimensional Partial Covariance Mass Spectrometry Open
Combinatorial post-translational modifications (PTMs), such as those forming the so-called "histone code", have been linked to cell differentiation, embryonic development, cellular reprogramming, aging, cancers, neurodegenerative disorders…
View article: Effect of the shot-to-shot variation on charge migration induced by sub-fs x-ray free-electron laser pulses
Effect of the shot-to-shot variation on charge migration induced by sub-fs x-ray free-electron laser pulses Open
X-ray free-electron lasers (XFELs) are now able to provide tunable pairs of intense sub-fs pulses in the soft x-ray regime, paving the way for time-resolved investigations of attosecond charge migration in molecules. However, the stochasti…