Separating the Good
from the Bad of X
Rays
|
The underlying control mechanism is the light-induced creation of coherence
between eigenstates of electrons in a material. This means that,
for a two-state system, light forces electrons to exist in both
states simultaneously rather than in one state or the other. This
light–matter
system can have fundamentally different properties from the matter
system in isolation, properties that can be controlled by varying
the properties of the optical control beam. Problems arise, however,
when the probe pulse lies in the x-ray regime because x rays interact
most strongly with the tightly bound (core) electrons in a material, leaving
behind a "core hole" that
is rapidly filled by more weakly bound electrons, thereby disrupting
the optically imposed coherence and destroying the control.
Similar disruptive events occur for visible probe pulses, but the key difference
for x-ray interactions is that the disruptive events occur about
a thousand times more rapidly than for visible-light interactions.
While the problems associated with a short coherence time can be
mitigated by using very intense optical control pulses, the high intensity
creates a different set of scientific problems. New technical problems also
arise. For example, ultrashort optical pulses are needed to achieve high
intensity and the x-ray pulse duration should be matched to the
optical pulse duration, thereby requiring femtosecond x-ray pulses.
To address this issue, the Berkeley Lab–Argonne team collaborated
on a series of experiments at ALS Beamline
6.0.2, which offers femtosecond-duration x-ray pulses and is one of
only a handful of places worldwide where the experiment could be
done. In the experiment, an intense femtosecond optical pulse co-propagated
with a femtosecond x-ray (~900-eV) pulse through a neon-filled
gas cell. Without the optical pulse, x rays were heavily attenuated
by the neon gas, but with it, the x-ray transmission increased
dramatically (by about a factor of three). The transparent window
created by the light pulse lasted just 70 fs, short enough to be
used to characterize x rays on ultrashort time scales. For example,
the research team used this window to measure the duration of a
femtosecond x-ray pulse, a heretofore difficult challenge. This
capability should help to further develop ultrafast x-ray spectroscopy.

ALS femtosecond spectroscopy beamline
layout. Femtosecond x-ray and laser pulses derive from a single
800-nm laser oscillator. Femtosecond x rays result from the interaction
of a laser pulse with an electron bunch as it passes through
the first of two insertion devices (the e-beam modulator) followed
by the passage of the modified bunch through the second insertion
device (the x-ray radiator), a technique known as laser
slicing. Control-laser pulses (70–300 fs) are focused to attain
the required intensity (~1013 W/cm2). A waveplate
and delay stage regulate the polarization and delay of the laser
pulses relative to the x-ray pulses. The x-ray and laser pulses
co-propagate through the neon sample gas cell.

Optically induced x-ray transparency data for
three peak laser intensities and a neon gas target with a thickness
of 108 torr-cm. The laser (~1.55 eV) coherently couples core-excited 3s
and 3p states, thereby inducing transparency on the 1s → 3p
x-ray absorption resonance. At the highest intensity (top), the
transmission increased by a factor of three relative to the transmission
at the lowest intensity. The solid lines show theoretical simulations
of the expected change in transmission. The degree of transparency
varies linearly with intensity within error.
Future research will focus on using similarly transparent windows to shape
x-ray pulses on a femtosecond time scale, a capability that opens
the door to new areas of x-ray research such as quantum control
of chemical reactions, a discipline now well developed in the visible
regime, where shaped pulses are used to control the evolution of
chemical reactions. It also lays a foundation for investigating
a broader spectrum of ways to use light to control how x rays interact with
matter. One interesting possibility is using light to enhance cross sections
for nonlinear x-ray scattering. Developing nonlinear spectroscopy in the
x-ray regime is currently hampered by weak cross sections for nonlinear
x-ray scattering.
Research conducted by T.E. Glover, M.P. Hertlein, and B. Rude (ALS); J.
van Tilborg and A. Belkacem (Berkeley Lab); S. Southworth, E.P. Kanter,
B. Krässig, H. Varma, and L. Young (Argonne National Laboratory); T.K.
Allison (Berkeley Lab and University of California, Berkeley); and R. Santra
(Argonne National Laboratory and University of Chicago).
Research funding: U.S. Department of Energy, Office of Basic Energy Sciences
(BES). Operation of the ALS is supported by BES.
Publication about this research: T.E. Glover, M.P. Hertlein, S.H.
Southworth, T.K. Allison, J. van Tilborg, E.P. Kanter, B. Krässig,
H.R. Varma, B. Rude, R. Santra, A. Belkacem, and L. Young, "Controlling
x-rays with light," Nature Physics 6, 69 (2009). |