380 research outputs found
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
Experimental Verification of the Chemical Sensitivity of Two-Site Double Core-Hole States Formed by an X-ray FEL
We have performed X-ray two-photon photoelectron spectroscopy (XTPPS) using
the Linac Coherent Light Source (LCLS) X-ray free-electron laser (FEL) in order
to study double core-hole (DCH) states of CO2, N2O and N2. The experiment
verifies the theory behind the chemical sensitivity of two-site (ts) DCH states
by comparing a set of small molecules with respect to the energy shift of the
tsDCH state and by extracting the relevant parameters from this shift.Comment: 11 pages, 2 figure
Femtosecond X-ray-induced fragmentation of fullerenes
A new class of femtosecond, intense, short – wavelength lasers – the free-electron laser – has opened up new opportunities to investigate the structure and dynamics in many scientific areas. These new lasers, whose performance keeps increasing, enable the understanding of physical and chemical changes at an atomic spatial scale and on the time scale of atomic motion which is essential for a broad range of scientific fields. We describe here the interaction of fullerenes in the multiphoton regime with the Linac Coherent Light Source (LCLS) X-ray free-electron laser at SLAC National Laboratory. In particular, we report on new data regarding the ionization of Ho3N@C80 molecules and compare the results with our prior C60 investigation of radiation damage induced by the LCLS pulses. We also discuss briefly the potential impact of newly available instrumentation to physical and chemical sciences when they are coupled with FELs as well as theoretical calculations and modeling
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
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