34 research outputs found
High-repetition-rate and high-photon-flux 70 eV high-harmonic source for coincidence ion imaging of gas-phase molecules
Unraveling and controlling chemical dynamics requires techniques to image
structural changes of molecules with femtosecond temporal and picometer spatial
resolution. Ultrashort-pulse x-ray free-electron lasers have significantly
advanced the field by enabling advanced pump-probe schemes. There is an
increasing interest in using table-top photon sources enabled by high-harmonic
generation of ultrashort-pulse lasers for such studies. We present a novel
high-harmonic source driven by a 100 kHz fiber laser system, which delivers
10 photons/s in a single 1.3 eV bandwidth harmonic at 68.6 eV. The
combination of record-high photon flux and high repetition rate paves the way
for time-resolved studies of the dissociation dynamics of inner-shell ionized
molecules in a coincidence detection scheme. First coincidence measurements on
CHI are shown and it is outlined how the anticipated advancement of fiber
laser technology and improved sample delivery will, in the next step, allow
pump-probe studies of ultrafast molecular dynamics with table-top XUV-photon
sources. These table-top sources can provide significantly higher repetition
rates than the currently operating free-electron lasers and they offer very
high temporal resolution due to the intrinsically small timing jitter between
pump and probe pulses
High-Gain Harmonic Generation with temporally overlapping seed pulses and application to ultrafast spectroscopy
Collinear double-pulse seeding of the High-Gain Harmonic Generation (HGHG)
process in a free-electron laser (FEL) is a promising approach to facilitate
various coherent nonlinear spectroscopy schemes in the extreme ultraviolet
(XUV) spectral range. However, in collinear arrangements using a single
nonlinear medium, temporally overlapping seed pulses may introduce nonlinear
mixing signals that compromise the experiment at short time delays. Here, we
investigate these effects in detail by extending the analysis described in a
recent publication (Wituschek et al., Nat. Commun., 11, 883, 2020). High-order
fringe-resolved autocorrelation and wave-packet interferometry experiments at
photon energies > eV are performed, accompanied by numerical simulations.
It turns out that both the autocorrelation and the wave-packet interferometry
data are very sensitive to saturation effects and can thus be used to
characterize saturation in the HGHG process. Our results further imply that
time-resolved spectroscopy experiments are feasible even for time delays
smaller than the seed pulse duration.Comment: This is accepted version of the article. The Version of Record is
available online at https://doi.org/10.1364/OE.40124
Electronic Quantum Coherence in Glycine Molecules Probed with Ultrashort X-ray Pulses in Real Time
Structural changes in nature and technology are driven by charge carrier
motion. A process such as charge-directed reactivity that can be operational in
radiobiology is more efficient, if energy transfer and charge motion proceeds
along well-defined quantum mechanical pathways keeping the coherence and
minimizing dissipation. The open question is: do long-lived electronic quantum
coherences exist in complex molecules? Here, we use x-rays to create and
monitor electronic wave packets in the amino acid glycine. The outgoing
photoelectron wave leaves behind a positive charge formed by a superposition of
quantum mechanical eigenstates. Delayed x-ray pulses track the induced
electronic coherence through the photoelectron emission from the sequential
double photoionization processes. The observed sinusoidal modulation of the
detected electron yield as a function of time clearly demonstrates that
electronic quantum coherence is preserved for at least 25 femtoseconds in this
molecule of biological relevance. The surviving coherence is detected via the
dominant sequential double ionization channel, which is found to exhibit a
phase shift as a function of the photoelectron energy. The experimental results
agree with advanced ab-initio simulations.Comment: 54 pages, 11 figure
Coherent superposition of two rotational states of carbon monoxide: Tracing a quantum rotor in space and time
We introduce a time-domain approach to explore rotational dynamics caused by intramolecular coupling or the interaction with dissipative media. It pushes the time resolution toward the ultimate limit determined by the rotational period. Femtosecond pulses create a coherent superposition of two rotational states of carbon monoxide. The wave-packet motion is observed by subsequent Coulomb explosion, which results in a time-dependent asymmetry of spatial fragmentation patterns. The asymmetry oscillation prevails for at least 1 ns, covering more than 300 periods with no decoherence. Long time scans will allow weak perturbations of the order of \Delta E/E=10^{−4} to be discerne
XUV fluorescence as a probe of laser-induced helium nanoplasma dynamics
XUV fluorescence spectroscopy provides information on energy absorption and dissipation processes taking place in the interaction of helium clusters with intense femtosecond laser pulses. The present experimental results complement the physical picture derived from previous electron and ion spectroscopic studies of the generated helium nanoplasma. Here, the broadband XUV fluorescence emission from high-lying Rydberg states that covers the spectral region from at 53.0 eV all the way to photon energies corresponding to the ionization potential of He ions at 54.4 eV is observed directly. The cluster size-dependent population of these states in the expanding nanoplasma follows the well-known bottleneck model. The results support previous findings and highlight the important role of Rydberg states in the energetics and dynamics of laser-generated nanoplasma
Attosecond Interferometry with Self-Amplified Spontaneous Emission of a free-electron laser
Light-phase-sensitive techniques, such as coherent multidimensional spectroscopy, are well-established in a broad spectral range, already spanning from radio-frequencies in nuclear magnetic resonance spectroscopy to visible and ultraviolet wavelengths in nonlinear optics with table-top lasers. In these cases, the ability to tailor the phases of electromagnetic waves with high precision is essential. Here we achieve phase control of extreme-ultraviolet pulses from a free-electron laser (FEL) on the attosecond timescale in a Michelson-type all-reflective interferometric autocorrelator. By varying the relative phase of the generated pulse replicas with sub-cycle precision we observe the field interference, that is, the light-wave oscillation with a period of 129 as. The successful transfer of a powerful optical method towards short-wavelength FEL science and technology paves the way towards utilization of advanced nonlinear methodologies even at partially coherent soft X-ray FEL sources that rely on self-amplified spontaneous emission
Split-and-delay Unit for FEL Interferometry in the XUV Spectral Range
In this work we present a reflective split-and-delay unit (SDU) developed for interferometric time-resolved experiments utilizing an (extreme ultraviolet) XUV pump–XUV probe scheme with focused free-electron laser beams. The developed SDU overcomes limitations for phase-resolved measurements inherent to conventional two-element split mirrors by a special design using two reflective lamellar gratings. The gratings produce a high-contrast interference signal controlled by the grating displacement in every diffraction order. The orders are separated in the focal plane of the focusing optics, which enables one to avoid phase averaging by spatially selective detection of a single interference state of the two light fields. Interferometry requires a precise relative phase control of the light fields, which presents a challenge at short wavelengths. In our setup the phase delay is determined by an in-vacuum white light interferometer (WLI) that monitors the surface profile of the SDU in real time and thus measures the delay for each laser shot. The precision of the WLI is 1 nm as determined by optical laser interferometry. In the presented experimental geometry it corresponds to a time delay accuracy of 3 as, which enables phase-resolved XUV pump–XUV probe experiments at free-electron laser (FEL) repetition rates up to 60 Hz
Attosecond Interferometry with Self-Amplified Spontaneous Emission of a free-electron laser
Light-phase-sensitive techniques, such as coherent multidimensional spectroscopy, are well-established in a broad spectral range, already spanning from radio-frequencies in nuclear magnetic resonance spectroscopy to visible and ultraviolet wavelengths in nonlinear optics with table-top lasers. In these cases, the ability to tailor the phases of electromagnetic waves with high precision is essential. Here we achieve phase control of extreme-ultraviolet pulses from a free-electron laser (FEL) on the attosecond timescale in a Michelson-type all-reflective interferometric autocorrelator. By varying the relative phase of the generated pulse replicas with sub-cycle precision we observe the field interference, that is, the light-wave oscillation with a period of 129 as. The successful transfer of a powerful optical method towards short-wavelength FEL science and technology paves the way towards utilization of advanced nonlinear methodologies even at partially coherent soft X-ray FEL sources that rely on self-amplified spontaneous emission
Femtosecond dynamics of correlated many-body states in fullerenes
In this joint theoretical and experimental work we investigate the population and decay dynamics of excited states of the C molecule by time-resolved two-photon photoemission. We map out how the thermally excited vibrational degrees of freedom lead to a transient redistribution of the photo-excited states. This includes the super-atom molecular orbitals (SAMOs), which are of great interest currently. The measured lifetimes are in line with full-fledged first-principle calculations