231 research outputs found
Optimisation of Quantum Trajectories Driven by Strong-field Waveforms
Quasi-free field-driven electron trajectories are a key element of
strong-field dynamics. Upon recollision with the parent ion, the energy
transferred from the field to the electron may be released as attosecond
duration XUV emission in the process of high harmonic generation (HHG). The
conventional sinusoidal driver fields set limitations on the maximum value of
this energy transfer, and it has been predicted that this limit can be
significantly exceeded by an appropriately ramped-up cycleshape. Here, we
present an experimental realization of such cycle-shaped waveforms and
demonstrate control of the HHG process on the single-atom quantum level via
attosecond steering of the electron trajectories. With our optimized optical
cycles, we boost the field-ionization launching the electron trajectories,
increase the subsequent field-to-electron energy transfer, and reduce the
trajectory duration. We demonstrate, in realistic experimental conditions, two
orders of magnitude enhancement of the generated XUV flux together with an
increased spectral cutoff. This application, which is only one example of what
can be achieved with cycle-shaped high-field light-waves, has farreaching
implications for attosecond spectroscopy and molecular self-probing
Photoionization in the time and frequency domain
Ultrafast processes in matter, such as the electron emission following light
absorption, can now be studied using ultrashort light pulses of attosecond
duration (s) in the extreme ultraviolet spectral range. The lack of
spectral resolution due to the use of short light pulses may raise serious
issues in the interpretation of the experimental results and the comparison
with detailed theoretical calculations. Here, we determine photoionization time
delays in neon atoms over a 40 eV energy range with an interferometric
technique combining high temporal and spectral resolution. We spectrally
disentangle direct ionization from ionization with shake up, where a second
electron is left in an excited state, thus obtaining excellent agreement with
theoretical calculations and thereby solving a puzzle raised by seven-year-old
measurements. Our experimental approach does not have conceptual limits,
allowing us to foresee, with the help of upcoming laser technology, ultra-high
resolution time-frequency studies from the visible to the x-ray range.Comment: 5 pages, 4 figure
Attosecond timing of electron emission from a molecular shape resonance
Shape resonances in physics and chemistry arise from the spatial confinement
of a particle by a potential barrier. In molecular photoionization, these
barriers prevent the electron from escaping instantaneously, so that nuclei may
move and modify the potential, thereby affecting the ionization process. By
using an attosecond two-color interferometric approach in combination with high
spectral resolution, we have captured the changes induced by the nuclear motion
on the centrifugal barrier that sustains the well-known shape resonance in
valence-ionized N. We show that despite the nuclear motion altering the
bond length by only , which leads to tiny changes in the potential
barrier, the corresponding change in the ionization time can be as large as
attoseconds. This result poses limits to the concept of instantaneous
electronic transitions in molecules, which is at the basis of the Franck-Condon
principle of molecular spectroscopy.Comment: 24 pages, 5 figure
Feasibility study of the National Autistic Society EarlyBird parent support programme
The EarlyBird programme is a group-based psychoeducation intervention for parents of young children with autism. Although it is widely used in the United Kingdom, the evidence base for the programme is very limited. Using a mixed method, non-randomised research design, we aimed to test (1) the acceptability of the research procedures (recruitment, retention, suitability of measures), (2) the parental acceptability of EarlyBird (attendance, views of the programme, perceived changes) and (3) the facilitator acceptability of EarlyBird (fidelity, views of the programme, perceived changes). Seventeen families with a 2- to 5-year-old autistic child and 10 EarlyBird facilitators took part. Pre- and post-intervention assessment included measures of the child’s autism characteristics, cognitive ability, adaptive behaviour, emotional and behavioural problems and parent-reported autism knowledge, parenting competence, stress and wellbeing. Semi-structured interviews were completed at post-intervention with parents and facilitators. For those involved in the study, the research procedures were generally acceptable, retention rates were high and the research protocol was administered as planned. Generally, positive views of the intervention were expressed by parents and facilitators. Although the uncontrolled, within-participant design does not allow us to test for efficacy, change in several outcome measures from pre- to post-intervention was in the expected direction. Difficulties were encountered with recruitment (opt-in to the groups was ~56% and opt-in to the research was 63%), and strategies to enhance recruitment need to be built into any future trial. These findings should be used to inform protocols for pragmatic, controlled trials of EarlyBird and other group-based interventions for parents with young autistic children
Acetylacetone photodynamics at a seeded freeelectron laser
The first steps in photochemical processes, such as photosynthesis or animal vision, involve changes in electronic and geometric structure on extremely short time scales. Time-resolved photoelectron spectroscopy is a natural way to measure such changes, but has been hindered hitherto by limitations of available pulsed light sources in the vacuum-ultraviolet and soft Xray spectral region, which have insufficient resolution in time and energy simultaneously. The unique combination of intensity, energy resolution, and femtosecond pulse duration of the FERMI-seeded free-electron laser can now provide exceptionally detailed information on photoexcitation–deexcitation and fragmentation in pump-probe experiments on the 50- femtosecond time scale. For the prototypical system acetylacetone we report here electron spectra measured as a function of time delay with enough spectral and time resolution to follow several photoexcited species through well-characterized individual steps, interpreted using state-of-the-art static and dynamics calculations. These results open the way for investigations of photochemical processes in unprecedented detail
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