E. Wigner first derived the general threshold laws for the dissociation
of a target into a pair of particles in 1948. In single-electron
photodetachment of negative ions where the reaction products (a
neutral atom and an electron) interact only in a short-range potential
(proportional to 1/r4), the threshold behavior is governed by the
centrifugal potential—the potential formed by the relative
angular momentum of the products—and depends only on the
energy (ε) and the relative angular momentum (l)
of the particles through εl+1/2.
He+-production cross section for 1s photodetachment from He–
closely follows a Wigner p-wave (l = 1) threshold
law (ε3/2), despite significant post-collision interaction
(PCI) effects. PCI appears only to effectively shift the observed
threshold position (arrow) by about 25 meV from the theoretical
position (vertical dashed line).
This form of the Wigner law has been observed in countless studies,
most notably in photodetachment of an outer (valence) electron
from negative ions. However, when an inner-shell electron is removed,
the neutral atom formed is unstable and quickly emits a second
electron (Auger decay). If one considers the final reaction products
to be two electrons and a positive ion, the short-range potential
threshold law would no longer apply. To investigate whether this
is so, the group studied inner-shell photodetachment in two negative
ions: He– and S–. The experimenters
monitored the photodetachment by measuring the positive ion yield
(He+, S+,
S2+, and S3+) at
the Ion-Photon Beamline on ALS Beamline 10.0.1
The ground-state electron configuration of He– is 1s2s2p.
For inner-shell photodetachment, the 1s electron is removed. Since
the electron gains one unit of angular momentum by absorbing the
photon, the receding photoelectron has angular momentum l =
1 and, in absence of Auger decay, one would expect a p-wave
threshold law: ε3/2. In fact, the measured near-threshold
cross section agrees very well with the p-wave law, except that
it is shifted in energy by a significant amount—i.e., the
Auger decay appears to mainly have the effect of requiring more
energy for the photodetached electron to escape. This can be understood
in the context of a post-collision interaction effect. Before the
photoelectron can fully escape, there is a chance that an Auger
process occurs and the fast Auger electron overtakes the slow photoelectron,
thus causing the photoelectron to be attracted and possibly recaptured
to the suddenly exposed positive core, so that the He+ signal is
suppressed.
Post-collision interaction with recapture is responsible for
shifting the observed He– threshold energy. Shortly after
the 1s electron in He– is photodetached, the atom ejects
a second electron in an Auger decay process (a). The high-energy
Auger electron quickly overtakes the photoelectron (b) which then
sees the exposed He nucleus (c) and can finally be recaptured (d)
to form a neutral He atom (shown in an excited state), which does
not contribute to the He+ signal monitored in these experiments.
To investigate the effect of the angular momentum l,
photodetachment of the 2p electron from S– was also studied. In
this case the absorption of the photon will cause the photoelectron
to leave with l = 1 ± 1 = 0 or 2, i.e., an s-wave
or d-wave. The d-wave component has always been too weak
to be observed, and the s-wave threshold law should be
expected: ε1/2. However, the group observed a change in
threshold shape as the d-wave contribution grew.
Observed S2+ signal (S+ and S3+ production is similar) from the
photodetachment of a 2p electron from S–. The s-wave law
(ε1/2) is followed closely up to nearly 3 eV above the
threshold (solid curve), after which the inclusion of the weak
d-wave is necessary to extend the agreement (dashed curve). In
the inset, the s-wave component has been subtracted from the data
to make the d-wave law (ε5/2) apparent. The departure
beyond about 166 eV is likely due to the opening of additional
detachment channels.
Furthermore, the wide energy range of agreement of the threshold
law to the observed signal was unprecedented; the Wigner law has
previously been observed to apply only some 0.01 to 0.1 eV above
the threshold, compared to the nearly 3 eV in inner-shell photodetachment,
a finding that is surprising and remains unexplained. Also surprising
is that this range of agreement was further improved with the inclusion
of a d-wave component to the fit. This is the first time a d-wave
has been observed in this way.
Research conducted by R. C. Bilodeau (Western Michigan University
and ALS); J.D. Bozek and G.D. Ackerman (ALS); N. D. Gibson and
C.W. Walter (Denison University); I. Dumitriu and N. Berrah (Western
Michigan University).
Research Funding: U.S. Department of Energy, Office of Basic Energy
Sciences (BES). Operation of the ALS is supported by BES.
Publications about this research:
R.C. Bilodeau, J.D. Bozek, N.D.
Gibson, C.W. Walter, G.D. Ackerman, I. Dumitriu, and N. Berrah, “Inner-shell
photodetachment thresholds: Unexpected long-range validity of the
Wigner law,” Phys. Rev. Lett. 95,
083001 (2005);
R.C. Bilodeau, N.D. Gibson, J.D. Bozek, C.W.
Walter, G.D. Ackerman, P. Andersson, J.G. Heredia, M. Perri, and
N. Berrah, “High-charge-state formation following inner-shell
photodetachment from S–,” Phys. Rev.
A 72,
050701(R) (2005);
R.C. Bilodeau, J.D. Bozek, G.D. Ackerman, A.
Aguilar, and N. Berrah, “Photodetachment of He– near
the 1s threshold: Absolute cross-section measurements and postcollision
interactions,” Phys. Rev. A 73,
034701 (2006).
ALSNews Vol. 263, March 29, 2006 |