Angular Distributions in Xenon
When light interacts with matter, it normally passes through (or is absorbed
or scattered by) the material; but, if the light is high intensity (> 10), then the light actually changes the matter it
is interacting with. For more information on this, see our
page on High Intensity Light-Matter Interactions. If the Light is intense
enough, the light will actually rip off the electrons of the atoms it is
interacting with. When this occurs, the ripped-off electron absorbs upwards
of 45 - 50 photons all at once. This normally happens in two steps: First,
the electron absorbs enough photons (thus gaining enough energy) to be
excited into a high-lying Rydberg state. Next, the electron will absorb
another number of photons and leave the atom with a certain amount of kinetic
energy. If the electron absorbs only one photon after being in the excited
state, the process is called Multi-Photon Ionization (MPI) since the electron
is just barely ionized. If the electron absorbs more than one electron
after being in the excited state, the process is called Above-Threshold
Ionization (ATI) since the electron has absorbed more photons above the
minimum energy it needed to be ionized. For more information on MPI and
ATI, see our
page on MPI and ATI.
For this experiment, we shined High Intensity, Short-Pulsed laser light
on Xenon. The light is generated from pumping a Ti:Sapphire crystal; the
light emitted is 800 nm in wavelength. To obtain high intensities, we generate
short pulses of light. Each pulse is approximately 110 fs (thats 1.1 x
10 s). Each pulse can have up to 850 mJ of energy
and our repetition rate is 1 kHz. The pressure in our chamber is adjusted
to be high enough to get fairly good signal-to-noise ratios yet low enough
to avoid space-charge effects. Our focused-down intensities are upwards
of 10. Below is a typical spectrum.
Note that the laser polarization angle for this spectrum is 0 degrees.
An explanation of polarization angle now follows. Our experiment is set
up such that the laser beam enters (and exits) a vacuum chamber (backing
pressure is approximately 4 x 10 torr). The
chamber is filled (to small pressures) with Xenon. The electrons we observe
travel perpendicularly to the laser pulses down a flight-tube to our Micro-Channel
Plate (MCP) detector. Now, if the electric field of the laser points in
the same direction of the flight tube, this is 0 degrees polarization.
The bulk of the electrons are ionized in this direction (and 180 degrees
from there). By passing the laser beam through a Half-Wave Plate, we can
turn the polarization through whichever angles we choose. When the polarization
of the electric field is perpendicular to the flight tube, this is 90 degrees
polarization; for certain intensities, we even see electrons at 90 degrees!

For this set of experiments in particular we are intested in how a spectrum
changes with a change in angle. Below is an example. If we just look at
at the 5g peak in the MPI order, we can display a radial plot of how the
peak height changes with respect to angle. The blue diamonds are our data
points, and the red line is a fit to our data using the scheme talked about
below.
As you can see, the distribution is not simply "all of the electrons come
out at 0 degrees". In fact, there are "jets" of electrons that come out
at 36 degrees and 72 degrees. Now, what exactly does this mean? Well, it
just so happens that one can model this system such that the data can be
fit with a sum of even (subscripted by 2L) Legendre Polynomials. The subscript
of the polynomials, L, according to the model, are related to the quantum
angular momenta of the electrons when they are in the Rydberg State (the
intermediate state in which they exist just before they are fully ionized).
Actually, a backwards fit needs to be done to figure out how the terms
in the 2L-Legendre Polynomials correspond to the coefficients of the "proper"
expansion. The reason we use this expansion is that when we combine all
the terms of the physically meaningful sum, the coefficients are all inter-related,
which make it difficult for fitting routines to handle. On the other hand,
the expansion we are currently using is also correct, just not as physically
meaningful -- and, since no terms share coefficients with each other, fitting
routines have an easy time fitting the data. In the future, we will work
backwards from the fits we have to the more physically meaningful terms.
In the meantime, there is some information we can get out of our fits.
Our fitting parameters do apply to physically meaningful quantities if
we assume no interference between Rydberg states. Below are shown, for
the fit above, which L's contribute to the angular momentum of the 4.3
x 10, 800 nm, 100 fs, MPI order
5g peak.
Evidently, there is a lot going on here. Mainly, we have a bunch of L=5,
with a good bit of L=0, 1, and 2 and a bit less of 3, 4, and 6. If, as
stated earlier, we assume no interferneces, we can see that having L=5
makes sense: the electron started in the L=4 (g) state, and absorbed one
photon, so there should be mostly L=5 (which there is). What is difficult
to see is why there exist bunches of the other terms. When we later work
back to the "meaningful" coefficients, that should shed some light ont
this. By then looking at what happens as we move from the 5g peak to the
6g peak to the 7g peak, &c. we can try to figure out better what the
mechanisms of ionization are and what processes are taking place. We can
also look from order to order to see how the distributions change. Another
way to look at the data is to look how the distributions change for a single
peak (say, the 5g of the MPI order) when we change the intensity.
Next, a word needs to be said regarding fitting the data and error bars.
Since our data comprise counted electrons, the percent uncertainty for
each point is 1/sqrt(Number of counts for that point). The horizontal error
bars are +/- 1¡. Since we have 16 data points for each plot, we fit
our data using 15 paramters so that we are neither critically nor over
parameterized. Below is the fit of the same data shown in the previous
two figures, where signal (normalized) is plotted vs. angle for the given
energy.
Plainly, the two jets seen in the radial plot up above are real, given
our error bars.
Finally, given the above data corresponding to a peak energy you may be
wondering how accurate our other, non-peak angular distributions are. Below
you will find a radial graph and its partner fitting plot, with error bars.
The specific energy value is 7.88 eV (for the same intensity as the above
graphs), which lies somewhere between photon orders; hence, the electron
counts here are smaller than those found at a peak energy.

One might argue that the 3rd, 4th, and 5th points from the left in the
data have an "uneeded" or "extra" bump present in the fit. However, even
if this "extra" bump were taken out, there would be some large feature
between those points that would stick out from the rest of the distribution.
The same can be said of those points near 40¡: here, a straight line
could
be drawn through them. Our fitting routine puts some minor bumps and wiggles
in those points, but no one can doubt that the main bumps/jets, near 20¡,
40¡, and 80¡ ought to be included in the fit.
The movies you can view show what happens to the angular distributions
when you keep the intensity the same, and scan in energy.
Page created by LVW Group. Last modified 3-Jun-98