Abstract

Total cross sections for double ionization of He and Li atoms by impact

of H
+
, He
2+
and Li
3+
were calculated at intermediate and high energies
within two-step models. Double ionization of He by impact of several
bare projectiles at xed energy were obtained as well. Single transition
probabilities were calculated within the continuum distorted wave eikonal-
initial-state (CDW-EIS) approximation. The optimized potential model
(OPM) was used to obtain atomic bound and unbound wavefunctions.
Correlation between events was introduced by considering the ion relax-
ation. The nal state electronic correlation was considered by means of
the so-called Gamow factor. We have found a good agreement with the
experimental results after the introduction of the relaxation eects and
inclusion of the nal state correlation.
1
Double ionization of atoms by fast ion impact:
two-step models
M.R. Fiori
y
, A. B. Rocha
z
, C.E. Bielschowsky
z
, Ginette Jalbert

and R. C. Garibotti

June 23, 2007

y
Departamento de Fsica, Universidad Nacional de Salta, Salta, Argentina
z
Instituto de Qumica, Departamento de Fsico-Qumica, Universidade Federal
do Rio de Janeiro, Rio de Janeiro, 21949-900, RJ, Brazil

Instituto de Fsica, Universidade Federal do Rio de Janeiro, Caixa Postal

68528, Rio de Janeiro, 21941-972, RJ, Brazil

Centro Atmico Bariloche and Instituto Balseiro, Comisin Nacional de En-

erga Atmica and Universidad Nacional de Cuyo, 8400 S. C. Bariloche, Ro
Negro, Argentina.
1 Introduction
Measurements of total cross sections for double ionization have been done for
dierent projectiles and targets in last decades, at high and intermediate ener-
gies. In particular, the double ionization of helium and lithium by impact of
H
+
, He
2+
and Li
3+
were measured by Shah et al [2, 3], as well as the ionization
of helium atom by impact of several bare ions at a x velocity by Knudsen et
al [4] and by McGuire et al [5].
The calculations of multiple ionization cross sections by charged particles
is a great challenge for theoretical physics. Dierent emission mechanisms are
possible, but it was recognized that the interaction of the projectile with each
electron is the dominant process at intermediate collision energies. This was de-
noted as the independent electron approximation (IEL) [6] and two-step model
or independent event model (IEV) [7]. In this interpretation, a multiple tran-
sition process must be described as a sequence of single electronic transition,
and the double ionization process has been treated as a succession of single
ionization processes by several authors in the context of distorted wave theories
[8, 9, 10, 11, 12, 13]. When the single ionization probabilities are evaluated,
both IEL and IEV models describe the general shape of the experimental total
double ionization cross sections but overestimate its absolute value as pointed
out by Bradley et al [13]. These models do not account for the electron-electron
correlation or the exclusion principle, that avoid to electrons to be emitted with
the same momenta. McCartney [12] introduced these constraints multiplying
2
the single probabilities by the continuum density of Coulomb states (CDS), also
denoted as the Gamow factor (G(/
12
)). With this factor, the IEL and IEV
models were called CDS-IEL and CDS-IEV model, respectively. Meanwhile the
magnitude of the theoretical cross sections given by the CDS-IEL model are too
large, the results given by the CDS-IEV model become comparable to data [13].
While our work was in progress, Bradley et al [13] published calculations of
the multiple ionization cross sections of helium, lithium and neon atoms by using
Roothan-Hartree-Fock (RHF) atomic functions for the initial state, and eective
charges 7
T
, for the nal ones, derived from the binding energies. They found
that the resulting probabilities for single ionization are larger than one at small
impact parametres, and propose a cutt-o and a decay methods to unitarize the
probabilties. They compare results obtained with the IEL and IEV approaches,
with and without the CDS factor, and found that the CDS-IEV agrees with
experiment at intermediate energies.
In this paper, we calculate the total double ionization cross sections for he-
lium and lithium atoms by impact of H
+
, He
2+
and Li
3+
in the context of the
two-step CDS-IEV model. This takes into account nal state electronic corre-
lation as well as the relaxation of the atom after the rst ionization event. The
individual probabilities were calculated within the CDW-EIS approximation of
Crothers and McCann [15] with numerically evaluated atomic wavefunctions for
the bound and continuum states. We solve the wave equation with the opti-
mized potential model (OPM) of Talman and Shadwick [16] avoiding the use of
parametric charges. As the initial state calculated from the RHF and the one
obtained from the OPM model are very similar, our approach is essentially the
same as Bradley et al [13], except for the choice of the nal wavefunction, that
we investigate the eect.
2 Theory
The probability 1(j. k) for a single atomic ionization event is related to a tran-
sition matrix T(:) by [11]:
1(j. k) = ja(j. k)j
2
=

Z
1
0
:d:J
0
(:j)
T(:. k)
2

2
. (1)
where a(j. k) is the probability amplitude, J
0
(r) the Bessel function, the
projectile velocity, : the transversal component of the transferred momentum
and k the electronic momentum. In this case one of the axis of the coordinate
system is in the direction. As was shown by Crothers and Holt [17] the
scattering amplitude is independent of the orientation of the vector in the
plane perpendicular to the projectile trajectory. Thus this plane may be chosen
as the collision plane without loss of generality. The single transition probability
1(j) is obtained as
1(j) =
Z
dkja(j. k)j
2
(2)
3
and the single ionization total cross section (SI) results:
o
SI
=
Z
jdj1(j) (3)
In the post version of the CDW-EIS approximation, the transition matrix is
given by
T
if
(:. k) =
D
.

\
y
f

.
+
i
E
. (4)
where .
+
i
is the initial eikonal distorted wavefunction,
.
+
i
= c
i
(x)1
+
i
(s. v) exp(iK
i
.R) (5)
with
c
i
(x) =
n
ni`i
r
1
mi
`i
(^r) (6)
where s, R, x are respectively the electron-projectile, projectile-nucleus and
atomic coordinates and K
i
is the initial momentum of the projectile in the
center of mass system. The nal Coulomb distorted wave is given by
.

f
= c

f
(x)1

f
(s. p) exp(i K
f
.R) (7)
with
c

f
(x) =
1
r
p
/
X
`m
i
`
exp(ic
`
)n
`k
(r) [1
m
`
(^r)]

1
m
`
(
^
k) (8)
where k is the momentum of the ejected electron in the target frame and
p = k v is the momentum of the electron in the projectile frame. The contin-
uum eigenstate c

f
(x) is normalized on the energy scale, with -
f
=
k
2
2
, through
the asymptotic unity ux condition.
We use a model potential to calculate the continuum and bounded electronic
wavefunctions for both the neutral and the ionized target. We have generated
this potential for the neutral helium and lithium atoms and ions with the opti-
mized potential model (OPM) of Talman and Shadwick [16]. In our calculations
for Hc, we set a OPM orbital energy of -
i
= 0.91795a.n. for the single ioniza-
tion energy, and the total double ionization energy is -
D
= 2.91795a.n., this is
consistent with the experimental values.
The double ionization of lithium atom may be produced by the ionization of
the two 1: electrons or by the ionization of one 1: and one 2: electron. In general,
the experimental results do not distinguish between these two possibilities and
the theoretical results model this process by a multinomial weight [18], having
in mind that the double ionization of two internal electrons 1: is much less
probable than the ionization of one 1: and one 2: electron. The code of Talman
[16] was used to calculate the discrete wavefunctions as well as the potentials
used to generate the continuum wavefunctions for the Li atom. The energies of
the orbitals considered in each type of calculations are presented in Table 1.
For the continuum wavefunctions, the radial Schrdinger equation was nu-
merically solved with the code of Salvat et al ([19]) using a logarithmic radial
4
Table 1: Energies of the orbitals -(1:), -(2:) for the litium atom and
-
D
= -(1:) + -(2:) considered in dierent models. Values were taken from
OPM code
Model -(1:) -(2:) -
D
IEL 2.0799 0.1962 2.2761
IEV1 2.7900 0.1962 2.9862
IEV2 2.0799 0.5922 2.6721
mesh j (see for details Ref. [20]). Numerical values of the transition matrix were
calculated for the dierent values of transversal transferred momentum (:), the
absolute value of the momentum (/) and the scattering angles of the momentum
of the ejected electrons with respect to the direction of the incident beam (0)
and with respect to the transversal transfered momentum (c). These values,
together with the radial mesh values (j), were chosen by the Gauss-Legendre
method.
After obtaining the wavefunction, we rst evaluated the transition matrix,
for the dierent events and a set of /, 0, c and j values. Then, we performed
numerical integrations to obtain the total cross section (DI) within a CDS-IEV
approximation:
o
DI
= 2
Z
dk
1
dk
2
jdjG(/
12
)1
A
1
(j. k
1
)1
A
+
2
(j. k
2
) (9)
3 Double ionization of helium atom: results and
discussion
In the two-step models (IEV), the value of the double ionization (DI) cross
sections is supposed to depend strongly on the quality of the model used in the
description of the single ionization (SI) cross sections . As a consequence, we
rst discuss the quality of our results for single ionization cross section.
In gure (1) we compare our calculations of the total cross section for sin-
gle ionization of helium by protons with the experimental results of Shah and
Gilbody [2]. The CDW-EIS approximation was used to describe the collision
process and the optimized potential model [16] to generate the discrete electronic
wavefunction for the He atom and continuum wavefunctions for the electron in
the eld of Hc
+
ion. The agreement between theory and experiments is ex-
cellent, diering by less than 10% in the interval of energy here considered.
For sake of completeness we also show the total cross sections for the single
ionization of He
+
ion by proton impact.
A notable feature in the present calculations can be observed by considering
the single ionization probabilities, as given by Eq.(2). In gure (2 (a)) we
show 1(j) for ionization of Hc by H
+
impact, for three energies in the range of
interest. We observe that the probabilities for electron emission from Hc by H
+
5
Figure 1: Total cross section for single ionization of He and He
+
by proton
impact as a function of the projectile energy 1
p
(in keV). Circles: experimental
results (Shah and Gilbody [2]); solid line: our calculated results.
Figure 2: Impact parameter dependent probabilites for single ionization of he-
lium by impact of (a) H
+
, (b) He
2+
, and (c) Li
3+
for dierent projectile energies.
Solid line: 50 keV; dashed line: 100 keV; dotted line: 300 keV; dot-dashed line:
1000 keV
impact are smaller than one. However this property is not preserved for Hc
2+
and 1i
3+
as can be observed in gure (2(b) and (c)), where the probabilties
are larger than one for small values of the impact parameter. This results from
the lack of unitarity of the CDW-EIS approach [21]. Bradley et al [13] have
proposed a cut-o and a damping procedures and shows that these reduces the
absolute value of the cross sections, for a Ne target. Fainstein [21] found that
the small impact parameters give a negligible contribution to the total single
o
SI
and double o
DI
cross sections. This is valid for high charge projectiles that
produce ionization even at large distances but, as can be observed in gure (
2(c)), the relevance of large j decreases as the projectile charge decreases.
In gure 3(a) we show the theoretical total cross sections for the double ion-
ization of the helium atom by protons, gure 3(b) by Hc
2+
and gure 3(c) by
1i
3+
. Our results can be compared with the experimental results of Shah and
Gilbody [2] and also with the theoretical CDS-IEV results of McCartney [22]
and et al [13]. These authors introduce an eective target charge in the nal
Coulomb waves of the emitted electrons, and McCartney found that results are
very sensitive to this value. The nal wavefunction that we have used results
from the numerical solution of the three-body equation with the experimen-
tal ionization energies and has not a parametric charge. For H
+
projectiles the
three approaches give equivalent results, but for Hc
2+
and 1i
3+
ions the present
method gives a maximum displaced to lower energies, in agreement with exper-
iments, but it is larger than the two other approaches, at intermediate energies.
OUr results present a good general agreement with experiments for the im-
pact of protons with energy between 200 and 1200 keV. In each single ionization
electrons emitted with low velocity relative to the atom or ion are dominant and
superposition of the continuum spectra of both electrons will be large, produc-
ing an strong correlation between electrons. Consequently, it is important to
consider accurately the electronic correlation. The Gamow factor is able to
describe correlation eects at intermediate energies, but produces an excessive
exponential inhibition to the emisssion of electrons with comparable velocities,
which constitute the majority of the emitted electrons at lower collision ener-
gies. Futhermore, as the Bohr parameter 7
P
increases the scattering event
may have sucient time for an enhanced correlation interactions between the
electrons, given place to a two-step-one mechanism (TS-1), sometimes called
knock-out (KO). This corresponds to the correlated dynamics of the two elec-
6
Figure 3: Total cross section for double ionization of helium atom by impact
of (a) H
+
, (b) He
2+
, and (c) Li
3+
as a function of the projectile energy 1
p
(in
keV/amu). Circles: experimental results of Shash and Gilbody ([2]); solid line:
our CDS-IEV results; squares: CDS-IEV result of McCartney ([22]).
Figure 4: Total cross section for double ionization of helium atom as a function
of the projectile charge (Z). Full circles: experimental results of McGuire et al
([5]); open circles: experimental results of Knudsen et al ([4]); solid line: our
CDS-IEV results; dot dashed line: theoretical results of Fainstein et al ([21]).
trons as they leave the atom where the primary electron is knocking out the
secondary electron. From gures we observe that these eects extend to higher
impact energies as the projectile charge increases. At high impact velocities the
contribution of rst order terms in 7
P
increases, these terms are associate
with a shake-o (SO) mechanism [8, 18] where an electron is emitted and the
second electron relaxes from an ionic bound state to continuum. These mecha-
nisms are not included in an independent electron description, which is of order
(7
P
)
2
.
It is important to point out that the dierences in the double ionization
cross sections for low impact energies of the projectile cannot be attributed to
the present description of the single ionization cross sections. Indeed, as pointed
out in gure 1, the single ionization cross sections are adequately described by
the CDW-EIS approach up to impact energies as low as 50 keV.
Another class of experiments was performed by Knudsen et al [4] and McGuire
et al [5] where for a He target the projectile energy was held xed at 1.44
MeV/amu and its charge was varied, allowing us to analyze the dependence
of the double ionization cross sections with the projectile charge. In gure 4),
theoretical results obtained by Fainstein et al [21] with the IEL approach are
larger than the presente ones.
4 Double ionization of lithiumatom: results and
discussion
The calculations of the double ionization cross sections for the Li atom within the
CDS-IEV (equation (9)) model may be done by three dierent ways, depending
on the order and nature of the two ionization steps considered: i) by considering
rst the ionization of the 2: electron and then, the ionization of the 1: electron
(C1); ii) by taking the inverse order, rst the ionization of the 1: electron and
then, the ionization of the 2: electron (C2) and nally, iii) by considering the
ionization of the two 1: electrons (C3). In the last case we do not consider
relaxation of the ionic wavefunction and the orbital energies are the same as
that of the neutral lithium.
In gure 5 we compare the present CDS-IEV double ionization cross sections
7
Figure 5: Total cross section for double ionization of lithium atom showing
the contribution of dierent processes. Solid line: ouor CDS-IEV (C1) results;
dashed line: our CDS-IEV (C2) results; dotted line: our double 1: ionization.
The numbers 1 or 2 refer to the sequence of events, see text
Figure 6: Total cross section for double ionization of lithium atom by impact of:
(a) H
+
and (b) He
2+
as a function of the projectile energy 1
p
(in keV/amu).
Circles: experimental results of Shash et al ([3]); solid line: our CDS-EIV (C1)
results; full squares: CDS-IEV results of McCartney([22])
of a Li atom for these three dierent situations. The emission alternatives C1
and C2 exhibit small dierences that reect the dependence of the two-step
model of the specic initial state, already found above. The experiments do
not distinguish between these two situations since the two ways lead to the
same nal state, formally theoretical results could be averaged. Figure 5 also
shows that the ionization of two 1: electrons (C3) presents a lower cross section
for low and intermediate impact energies indicating that this process does not
contribute signicantly to the total cross section. Therefore we have evaluate
the total cross section with the CDS-IEV approximation applying the sequence
denoted as C1. The results are shown in gure 6(a) and (b) for H
+
and Hc
2+
projectiles respectively, together with the experimental results of Shah et al [3]
and theoretical results of McCartney [22].
Cross sections show a good agreement with the experimental results for
impact energies between 150 and 1000 keV. For low and high energies the present
results deviate from the experimental cross sections, probably due to the knock-
out and shake-o processes respectively as discusses for He targets.
5 Conclusions
We have calculated the total cross sections for the double ionization of helium
and lithium atoms with dierent projectiles. The collision process was described
as two consecutive single ionization events, each evaluated with the continuum
distorted wave eikonal-initial-state approximation of Crothers and McCann [15].
The single ionization amplitudes were calculated by using numeric atomic wave-
functions obtained with OPM potentials.
We have considered an independent electron event model, where the double
ionization is produce through two distinct events, rst the single ionization of
the neutral atom and second, the single ionization of the ion. This is a two
step (TS2) mechanism that comes from the (7
P
)
2
order in a perturbative
expansion of the scattering amplitude. The correlation between the ionized
electrons was introduced with the Gamow factor. This accounts for both the
relaxation eects of the ion after the rst ionization and the correlation between
the ejected electrons.
8
We applied this method to the evaluation of total cross sections for double
ionization of Hc and 1i by H
+
,o Hc
2+
and 1i
3+
projectiles. Our results present
a general good agreement with experiments for intermediate impact energy be-
tween 200 keV and 1000 or 2000 keV, depending on the projectile charge. When
the projectile charge is increased wider the range of validity of the model.
We compare our results with former theoretical calculations of McCartney
[22] and Bradley et al [13]. The main dierence between the present calcula-
tions and those former works is in evaluation of the two electrons wavefunctions
relative to target. More specically, we used the OPM potential model while,
McCartney and Bradley et al used an eective charge potential for the nal
state and RHF waves for the initial states. As was shown in reference [20], the
total cross sections for single ionization are relatively insensitive to the atomic
nal wavefunctions but the dierential cross sections present greater dierences
between the cross sections calculated using these two approaches. In fact, the
OPM approach leads to better agreement than eective charge model when
compared to the experimental results for the dierential cross sections. The
optimized potential model (OPM) allows for a more accurate representation of
one electron orbitals than does the rather crude eective charge models.
For energies lower than 150 keV, the electron-electron correlation is not well
describe by the Gamow factor and the 7
P
rst order knock-out mechanism
increases his relevance. For higher impact energies, we believe that shake-o
processes, not considered in the present two-step calculations, may contribute
signicantly.
and FAPERJ and by CIUNSa (Salta-Argentina).
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