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An atom or molecule exposed to a high intensity
laser pulse becomes excited or eventually photoionized even if the
energy of the photons is much less than the ionization potential
and the first bound excited state of the system. With rising light
intensity even multiple ionization is observed and for molecules
in addition dissociation into charged fragments. In the long wavelength
limit the photoionization mechanism can well be understood in semicalssical
terms. Photoionization becomes electric field ionization in the
strong, oscillating electric field of the light pulse which easily
reaches inneratomic levels. Multiple ionization in such a light
pulse is usually not a succession of independent electric field
ionization steps where one electron after the other is removed.
It was found that they leave the atom in a highly correlated way
(see our
publication).
Experimental
access to strong field processes
The appropriate method to investigate the momentum
correlation of the photoelectrons and ions (for moleculular excitation)
is a complete analysis of the final momenta of all charged particles
(electrons and ions) formed after the interaction of the light pulse
with the atom or molecule. This gives detailed insight into the
mechanisms leading to excitation, multiple ionization and the mutual
interaction of the electrons and ions (their correlation) while
they leave the atom/molecule. Today, this analysis is usually done
with the help of a reaction microscope.
The Momentum Spectrometer (Reaction Microscope)

In the center of the reaction microscope a cold
supersonic atomic/molecular beam is intersected by a focused laser
beam. Ions and electrons created in the focal spot are extracted
by a weak homogenous electric field. At the end of two drift tubes
they reach position sensitive detectors. For each particle, electron
and ion, all three Cartesian components of the momentum it gained
in the interaction with the laser pulse can be reconstructed with
high accuracy from its time of flight and the position where it
hits the detector. The electric field together with a homogeneous
magnetic field for the photoelectrons is able to guide all charged
particles from the laser focal spot to the detectors.
The current
field of research: Strong field ionization of noble gas dimers
Why are noble gas dimers of interest?
| - They constitute
diatomic molecules with large internuclear separation (R ~ 3.5
- 4.5 Å) |
| - The molecule consists
of two nearly unperturbed atoms (weak polarization forces form
the bond) |
| - The
first ionization potential is nearly equal to that of the atomic
contituents |
| -
They practically form a double slit atomic electron emitter
(two-center interference of emitted electron waves)

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| - In the
singly charged ion electron charge oscillations can be induced
by the applied strong electric field of the laser pulse |
- Double
ionization (DI) may proceed via different pathways:
- two-site DI (followed by Coulomb explosion)
- one-site DI (followed by charge transfer and Coulomb exposion)
- one-site single ionization with excitation of a second
electron at the same site (followed by "interatomic
Coulombic decay" (ICD) or autoionization after charge
transfer)
- "frustrated" strong field triple ionization
(for "frustrated" tunnel ionization see T.
Nubbemeyer et al.)
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The "double slit"
strong field electron emitter
We have investigated the appearance of "double
slit" interference in the photoelectron spectra of Ar2
dimers after strong field single ionization. Due to the large internuclear
separation R of the dimer (R ~ 3.8 Å) interference appears
already in the spectrum of the directly emitted photoelectrons (which
did not rescatter on the dimer ion core) having small kinetic energy.
The first results can be found in Z.
Ansari et al..
Interference in the photoelectron spectrum only
appears provided it is principally impossible to localize the atomic
constituent of the dimer from which the electon was emitted. In
the case of the noble gas dimers this means the ion is formed in
a definite "gerade" or "ungerade"
state of a charge resonance pair of states. In this case the strong
field transition amplitude of the Ar2
dimer also in the strong field ionization limit can be written (at
least approximatly) as a product of the atomic transition amplitude
to the continuum and an interference term (see Z.
Ansari et al.). This allows an extraction of the contribution
of interference to the dimer photoelectron spectrum by simply dividing
the dimer by the atomic spectrum.
High resolution Ar2 and
Ar photoelectron momentum distributions are shown in the figure
below. The laser parameters are given in the figure. Distinct
differences between the atomic and dimer spectra are foung in the
vicinity of zero momentum. This localization of the differences
is mainly due to the fact that the dimer axis is not aligned with
respect to the direction of polarization of the laser beam.

In order to extact the contribution of two center
interference to the dimer spectrum we divide the spectra point wise
and extract cuts trough this spectrum along the pz-axis.
The result is shown in the next figure for three
cuts at different pr.

The smooth lines indicate fits to the experimental
interference factor assuming a certain distribution of the ion over
different accessible states with definit symmetry with respect to
inversion. Part of the momentum dependence of the ratios is well
reproduced by the fits. Mainly the "ungerade"
fraction of the charge resonance ionic states contributes thus allowing
interference in the photoelectron spectrum to appear since in this
case an identification of the emission center is in principle impossible.
Only a narrow spike in the ratio at zero momentum cannot be attributed
to two-slit inteference. This spike can also easily identified in
the dimer photoelectron spectrum above.
Present status:
- Two-slit interference is found in the photoelectron spectra
of all noble gas dimers (Ne2,
Ar2, Kr2,
and Xe2) after strong field ionization.
- It is more or less pronounced depending on whether the
atomic emission centers are indistiguishable (i. e. the
final ionic states reached have the same parity).
- Similar population of ionic charge resonance state pairs
with opposite parity extinguishes interference since then,
in principle, the atomic center that emitted the electron
is identifiable.
- The interference factor (ratio of the dimer and corresponding
atom photoelectron spectra) always shows a pronounced spike
at zero momentum.
- This spike, whose origin is presently not clear, does
not seem to be an interference phenomenon.
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For more details on the role of two-slit interference
in the photoelectron spectra of molecules at large internuclear
separation ionized by strong laser pulses see Z.
Ansari et al..
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