49 research outputs found
Interatomic-Coulombic-decay-induced recapture of photoelectrons in helium dimers
We investigate the onset of photoionization shakeup induced interatomic
Coulombic decay (ICD) in He2 at the He+*(n = 2) threshold by detecting two He+
ions in coincidence. We find this threshold to be shifted towards higher
energies compared to the same threshold in the monomer. The shifted onset of
ion pairs created by ICD is attributed to a recapture of the threshold
photoelectron after the emission of the faster ICD electron.Comment: 5 Pages, 2 Figure
A measurement of the evolution of Interatomic Coulombic Decay in the time domain
During the last 15 years a novel decay mechanism of excited atoms has been
discovered and investigated. This so called ''Interatomic Coulombic Decay''
(ICD) involves the chemical environment of the electronically excited atom: the
excitation energy is transferred (in many cases over long distances) to a
neighbor of the initially excited particle usually ionizing that neighbor. It
turned out that ICD is a very common decay route in nature as it occurs across
van-der-Waals and hydrogen bonds. The time evolution of ICD is predicted to be
highly complex, as its efficiency strongly depends on the distance of the atoms
involved and this distance typically changes during the decay. Here we present
the first direct measurement of the temporal evolution of ICD using a novel
experimental approach.Comment: 6 pages, 4 figures, submitted to PR
Vibrationally Resolved Decay Width of Interatomic Coulombic Decay in HeNe
We investigate the ionization of HeNe from below the He 1s3p excitation to
the He ionization threshold. We observe HeNe ions with an enhancement by
more than a factor of 60 when the He side couples resonantly to the radiation
field. These ions are an experimental proof of a two-center resonant
photoionization mechanism predicted by Najjari et al. [Phys. Rev. Lett. 105,
153002 (2010)]. Furthermore, our data provide electronic and vibrational state
resolved decay widths of interatomic Coulombic decay (ICD) in HeNe dimers. We
find that the ICD lifetime strongly increases with increasing vibrational
state.Comment: 7 pages, 5 figure
Recommended from our members
Charge transfer to ground-state ions produces free electrons
Inner-shell ionization of an isolated atom typically leads to Auger decay. In an environment, for example, a liquid or a van der Waals bonded system, this process will be modified, and becomes part of a complex cascade of relaxation steps. Understanding these steps is important, as they determine the production of slow electrons and singly charged radicals, the most abundant products in radiation chemistry. In this communication, we present experimental evidence for a so-far unobserved, but potentially very important step in such relaxation cascades: Multiply charged ionic states after Auger decay may partially be neutralized by electron transfer, simultaneously evoking the creation of a low-energy free electron (electron transfer-mediated decay). This process is effective even after Auger decay into the dicationic ground state. In our experiment, we observe the decay of Ne2+ produced after Ne 1s photoionization in Ne-Kr mixed clusters
Ion and Electron Momentum Distributions from Single and Double Ionization of Helium Induced by Compton Scattering
We present the momentum distributions of the nucleus and of the electrons from double ionization of the helium atom by Compton scattering of photons with hν=40  keV. We find that the doubly charged ion momentum distribution is very close to the Compton profile of the nucleus in the ground state of the helium atom, and the momentum distribution of the singly charged ion to give a precise image of the electron Compton profile. To reproduce these results, nonrelativistic calculations require the use of highly correlated initial- and final-state wave functions
Recommended from our members
Evidence for Efficient Pathway to Produce Slow Electrons by Ground-state Dication in Clusters
We present an experimental evidence for a so-far unobserved, but potentially very important step relaxation cascades following inner-shell ionization of a composite system: Multiply charged ionic states created after Auger decay may be neutralized by electron transfer from a neighboring species, producing at the same time a low-energy free electron. This electron transfer-mediated decay (ETMD) called process is effective even after Auger decay into the dicationic ground state. Here, we report the ETMD of Ne2+ produced after Ne 1s photoionization in Ne-Kr mixed clusters
Fourfold Differential Photoelectron Circular Dichroism
We report on a joint experimental and theoretical study of photoelectron circular dichroism (PECD) in methyloxirane. By detecting O 1s photoelectrons in coincidence with fragment ions, we deduce the molecule’s orientation and photoelectron emission direction in the laboratory frame. Thereby, we retrieve a fourfold differential PECD clearly beyond 50%. This strong chiral asymmetry is reproduced by ab initio electronic structure calculations. Providing such a pronounced contrast makes PECD of fixed-in-space chiral molecules an even more sensitive tool for chiral recognition in the gas phase
Photoelectron circular dichroism of O 1-photoelectrons of uniaxially oriented trifluoromethyloxirane: Energy dependence and sensitivity to molecular configuration
The photoelectron circular dichroism (PECD) of the O 1s-photoelectrons of
trifluoromethyloxirane(TFMOx) is studied experimentally and theoretically for
different photoelectron kinetic energies. The experiments were performed
employing circularly polarized synchrotron radiation and coincidentelectron and
fragment ion detection using Cold Target Recoil Ion Momentum Spectroscopy. The
corresponding calculations were performed by means of the Single Center method
within the relaxed-core Hartree-Fock approximation. We concentrate on the
energy dependence of the differential PECD of uniaxially oriented TFMOx
molecules, which is accessible through the employed coincident detection. We
also compare results for differential PECD of TFMOx to those obtained for the
equivalent fragmentation channel and similar photoelectron kinetic energy of
methyloxirane (MOx), studied in our previous work. Thereby, we investigate the
influence of the substitution of the methyl-group by the trifluoromethyl-group
at the chiral center on the molecular chiral response. Finally, the presently
obtained angular distribution parameters are compared to those available in
literature.Comment: 6 fig
Enantiosensitive Structure Determination by Photoelectron Scattering on Single Molecules
X-ray as well as electron diffraction are powerful tools for structure
determination of molecules. Electron diffraction methods yield
\r{A}ngstrom-resolution even when applied to large systems or systems involving
weak scatterers such as hydrogen atoms. For cases in which molecular crystals
cannot be obtained or the interaction-free molecular structure is to be
addressed, corresponding electron scattering approaches on gas-phase molecules
exist. Such studies on randomly oriented molecules, however, can only provide
information on interatomic distances, which is challenging to analyse in case
of overlapping distance parameters and they do not reveal the handedness of
chiral systems8. Here, we present a novel scheme to obtain information on the
structure, handedness and even detailed geometrical features of single
molecules in the gas phase. Using a loop-like analysis scheme employing input
from ab initio computations on the photoionization process, we are able to
deduce the three dimensional molecular structure with sensitivity to the
position individual atoms, as e.g. protons. To achieve this, we measure the
molecular frame diffraction pattern of core-shell photoelectrons in combination
with only two ionic fragments from a molecular Coulomb explosion. Our approach
is expected to be suitable for larger molecules, as well, since typical size
limitations regarding the structure determination by pure Coulomb explosion
imaging are overcome by measuring in addition the photoelectron in coincidence
with the ions. As the photoelectron interference pattern captures the molecular
structure at the instant of ionization, we anticipate our approach to allow for
tracking changes in the molecular structure on a femtosecond time scale by
applying a pump-probe scheme in the future