193 research outputs found
Macroscopic effects in attosecond pulse generation
We examine how the generation and propagation of high-order harmonics in a
partly ionized gas medium affect their strength and synchronization. The
temporal properties of the resulting attosecond pulses generated in long gas
targets can be significantly influenced by macroscopic effects, in particular
by the intensity in the medium and the degree of ionization. Under some
conditions, the use of gas targets longer than the absorption length can lead
to the generation of self-compressed attosecond pulses. We show this effect
experimentally, using long argon-filled gas cells as generating medium.Comment: 5 pages 4 figure
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
Photoemission time-delay measurements and calculations close to the 3s ionization minimum in Ar
We present experimental measurements and theoretical calculations of
photoionization time delays from the and shells in Ar in the photon
energy range of 32-42 eV. The experimental measurements are performed by
interferometry using attosecond pulse trains and the infrared laser used for
their generation. The theoretical approach includes intershell correlation
effects between the 3s and 3p shells within the framework of the random phase
approximation with exchange (RPAE). The connection between single-photon
ionization and the two-color two-photon ionization process used in the
measurement is established using the recently developed asymptotic
approximation for the complex transition amplitudes of laser-assisted
photoionization. We compare and discuss the theoretical and experimental
results especially in the region where strong intershell correlations in the 3s
to kp channel lead to an induced "Cooper" minimum in the 3s ionization
cross-section.Comment: submitted to PR
Photoemission-time-delay measurements and calculations close to the 3s-ionization-cross-section minimum in Ar
We present experimental measurements and theoretical calculations of photoionization time delays from the 3s and 3p shells in Ar in the photon energy range of 32-42 eV. The experimental measurements are performed by interferometry using attosecond pulse trains and the infrared laser used for their generation. The theoretical approach includes intershell correlation effects between the 3s and 3p shells within the framework of the random-phase approximation with exchange. The connection between single-photon ionization and the two-color two-photon ionization process used in the measurement is established using the recently developed asymptotic approximation for the complex transition amplitudes of laser-assisted photoionization. We compare and discuss the theoretical and experimental results, especially in the region where strong intershell correlations in the 3s -> kp channel lead to an induced "Cooper" minimum in the 3s ionization cross section
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