Literature Survey On M Shell
Literature Survey On M Shell
J. Phys. Chem. Ref. Data 50, 043106 (2021); https://doi.org/10.1063/5.0058390 50, 043106
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AFFILIATIONS
1
Department of Basic and Applied Sciences, Punjabi University, Patiala, 147002 Punjab, India
2
Department of Physics, Chandigarh University, Gharuan, Mohali-140413, Punjab, India
a)
Author to whom correspondence should be addressed: sanjivpurichd@yahoo.com
ABSTRACT
In the present work, the experimental total and line resolved M-series x-ray production cross sections (XRPCSs) for different elements with
Z = 59–92 for 0.05–39.34 MeV proton and 0.2–6.0 MeV He ion (3 He/4 He) impact reported by different research groups until December
2020 have been compiled in tabular form. A status of different physical parameters, namely, the ionization cross sections, x-ray emission
rates, fluorescence yields, and Coster–Kronig and super Coster–Kronig yields, required to calculate the theoretical M-series XRPCSs have
been reviewed. The tabulated experimental total M-series XRPCSs for different elements are found to exhibit universal scaling similar to that
shown by the theoretical cross sections. These tabulated experimental cross sections for different elements have been parameterized in order
to provide empirical cross sections for use in different applications.
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Key words: fluorescence and Coster-Kronig yields; M-series x-ray production cross sections; proton and helium ion induced M-series
x-ray emission; x-ray emission rates.
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have been parameterized in order to provide empirical cross sections transferred through the CK/SCK transitions and can be calculated
for use in different applications. using the equation
τ I τ
σMi = σMi + ∑k<i σMk f ki , (2)
2. Theoretical M-series XRPCSs
Radiative decay of the charged particle induced Mi (i = 1–5) where σMiI
represents the Mi (i = 1–5) sub-shell ionization cross
sub-shell vacancies results in emission of x-ray series comprising section for a given element at the specific projectile ion energy (E)
several lines in each case, as depicted in Fig. 1. Accordingly, the and fki denotes the Mi sub-shell CK/SCK yields. The total M-series
M5 sub-shell x-ray series includes the Mξ1(M5 –N3 ), Mα1 (M5 –N7 ), XRPCSs can be evaluated using the relation
Mα2 (M5 –N6 ), and (M5 –O3 ) x-ray lines; the M4 sub-shell x-ray series X
σMtot X
(E) = ∑j σMj . (3)
includes Mδ1 (M4 –N3 ), Mξ 2 (M4 –N2 ), Mβ(M4 –N6 ), (M4 –O2 ), and
(M4 –O3 ) lines; the M3 sub-shell series comprises the Mδ2 (M3 –N1 ), The XRPCSs are usually expressed in units of barns, where
(M3 –N2 ), (M3 –N4 ), Mγ (M3 –N5 ), Mm1 [(M3 –N6,7 )+ (M3 –O1 ) 1 b = 10−28 m2 . The total M-series XRPCSs can also be evaluated
+ (M3 –O4,5 )] lines; the M2 sub-shell series includes the Mm2 using the relation
[(M2 –N1 ) + (M2 –O1 ) + M2 –O4 )] and Mm1 (M2 –N4 ) lines; and the
X I
M1 sub-shell series includes theMm1 (M1 –N2,3 ) and Mm2 (M1 –O2,3 ) σMtot (E) = σM × ωM , (4)
x-ray lines. The theoretical Mj XRPCSs, σMj X
(j = ξ, δ, α, β, ζ, γ, m1 , I
m2 ), at a given projectile ion energy (E) can be calculated using the where σM represents the total M-shell ionization cross section and
relation ωM denotes the average M-shell fluorescence yields. The current sta-
X τ
tus of different Mi (i = 1–5) sub-shell physical parameters required
σMj (E) = σMi ωi Fij , (1) to calculate the M-series XRPCSs is discussed below.
where ωi represents the Mi (i = 1–5) sub-shell fluorescence yield
and Fij denotes the fractional emission rate for the Mj x-ray line 2.1. Charge particle induced Mi sub-shell ionization
originating from decay of the Mi sub-shell vacancy [Mi (i = 1, 2, 3), cross sections
j = m1 ; Mi (i = 1, 2), j = m2 ; M3 , j = γ; Mi (i = 4, 5), j = ξ; M5, j = α; In the literature, two theoretical approaches are available to
M3 , j = β; Mi (i = 3, 4), j = δ; and M2 , j = ζ ]. σMi
τ
denotes the total calculate the charged particle induced atomic inner-shell ioniza-
number of vacancies in the Mi (i = 1–5) sub-shell including those tion cross sections. The first approach pertains to the calculations
FIG. 1. Energy level diagram showing electron transitions allowed by selection rules (Δn ≥1, Δl = ±1, and Δj = 0, ±1) resulting in emission of different Mi (i = 1–5) sub-shell
x rays.
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TABLE 1. Comparison of the proton induced Mi (i = 1–5) sub-shell ionization cross sections based on the DHS model35,36 and the ECPSSR model37
% Difference between DHS,35,36 ECPSSR,33,34 and ECUSAR37,38 model based proton ionization cross sections
0.06 MeV 0.1 MeV 0.7 MeV 2.0 MeV
Shell/ Atomic DHS and DHS and DHS and DHS and DHS and DHS and DHS and DHS and
Sub-shell region ECPSSR ECUSAR ECPSSR ECUSAR ECPSSR ECUSAR ECPSSR ECUSAR
M1 55 ≤ Z ≤ 92 3–64 1–61 1–56 1–54 10–33 6–31 1–9 1–10
M2 55 ≤ Z ≤ 92 3–188 1–249 1–92 3–93 7–13 3–9 1–9 1–11
M3 55 ≤ Z ≤ 92 1–47 2–61 12–42 8–38 4–17 1–14 1–9 1–15
M4 55 ≤ Z ≤ 92 21–261 6–289 1–96 1–120 4–16 2–13 1–11 1–11
M5 55 ≤ Z ≤ 92 20–178 4–195 1–67 1–75 6–15 7–15 5–9 3–9
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≤ 92. The second set of these yields based on the DHS model cal-
culations were reported by Chen et al.48,49 These DHS model based
Mi (i = 1–3) sub-shell yields were reported49 for ten elements in the
atomic region 67 ≤ Z ≤ 95 and the Mi (i = 4, 5) sub-shell yields were
reported50 for eight elements in the atomic region 70 ≤ Z ≤ 100. In
recent past, a complete set of the DHS model based Mi (i = 1–5)
sub-shell fluorescence and CK/SCK yields for elements with 67
≤ Z ≤ 92 interpolated from available limited data48,49 considering the
cutoff and onset of different CK/SCK transitions were reported by
Chauhan and Puri.51 These authors obtained the information about
the cutoff/onset of different CK/SCK transitions from the energies
of these transitions evaluated using the Dirac–Hartree–Fock–Slater
(DHFS) model based neutral atom binding energies52 and the
Li (i = 1–3) sub-shell CK transition energies.53 Furthermore, the
average M-shell fluorescence yields (ωM ) have been tabulated by
Hubbell et al.54
Two sets of the Mi (i = 1–5) sub-shell ωi and fij values are com-
pared in Figs. 4 and 5, respectively, by plotting ratios of the DHS
model51 based values to the NRHS model based values47 as a func-
FIG. 3. Ratios of the DHS model35,36 based Mi (i = 1–5) sub-shell ionization cross tion of atomic number (Z). It is clear from Fig. 4 that two sets of the
sections to the ECUSAR model37,38 based values as a function of atomic number ωi (i = 1–5) yields based on the DHS model51 and NRHS model47
of the target element at three incident proton energies: (a) 0.06 MeV, (b) 0.7 MeV, calculations differ by 12%–63%. It is obvious from Figs. 5(a)–5(c)
and (c) 2.0 MeV.
that the two sets of the fij (i = 1, j = 2–5) values differ by 18%–52%;
the fij (i = 2, j = 3–5) values differ by 9%–29%; and the fij (i = 3, j
= 4, 5) values differ by 7%–34%. On the other hand, the f45 values
differ by up to 29%–62% for elements with Z = 81–84, and these
decay of the M3 /M4 /M5 sub-shell vacancies is expected to exhibit differences become enormous (up to a factor of two) for elements
alignment effects. The angular distribution of x rays emitted with Z = 74–78, whereas for the remaining elements in the inves-
from an aligned vacancy state can be described as (I(θ)/dΩ) tigated atomic region, these differences are found to be up to 13%
= (Io /4π)[1 + βP2 (cos θ)], where Io is the total x-ray intensity, θ is [Fig. 5(c)].
the angle of observation with respect to the incident beam direction,
P2 (cos θ) is the second order Legendre polynomial, and β (≡αA20 ) is 2.3. M-shell x-ray emission rates
called the anisotropy parameter of a particular line. Here, α is a con-
stant depending on the total angular momentum of the initial and The Mi (i = 1–5) sub-shell vacancy decay through a radiative
final state of the ionized atom, and A20 is the degree of alignment transition is characterized by the x-ray emission rate. The fractional
for a given sub-shell. The values of α have been given elsewhere.45 It
was shown by Sizov and Kabachnik46 that the alignment of atomic
inner-shell vacancies produced by proton impact is a function of the
projectile ion velocity and is large for low-velocity incident protons.
To the best of our knowledge, experimental investigations on the
charged particle induced Mi (i = 1–5) sub-shell vacancy alignment
are not available in the literature.
J. Phys. Chem. Ref. Data 50, 043106 (2021); doi: 10.1063/5.0058390 50, 043106-5
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FIG. 5. Ratios of the DHS model51 based Mi (i = 1–5) sub-shell CK yields and
those tabulated by McGuire:47 (a) f12 , f13 , f14 , f15 ; (b) f23 , f24 , f25 ; and (c) f34 , f35 ,
f45 for different elements with 67 ≤ Z ≤ 90. The dotted line is plotted to guide
the eye.
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the charge particles and ignoring the many-body effects, which are A scan of the available experimental data (Table 2) indicated a
expected to become important for heavy elements. However, the large scatter in the measured values for any given element at differ-
ion–atom collisions are known to produce simultaneous ioniza- ent incident proton energies and noticeable discrepancies between
tion in the outer atomic shells. For example, the 2.0 MeV helium measured and theoretical M-series XRPCSs. As an illustration, the
ions incident on a bismuth (Z = 83) target are found to create case of Au has been considered as it is the most investigated ele-
the K/L/M shell vacancies in the ratio 1.0:1.2 × 105 :6.2 × 108 , as ment for which 151 values of total M-series XRPCSs at differ-
evident from the ECUSAR model37,38 based ionization cross sec- ent proton energies ranging 0.05–39.34 MeV are available from 13
tions. The simultaneous presence of multiple vacancies in the atomic publications. In order to make comparisons between experimen-
shells (outer than the atomic shell/sub-shell of interest) results in tal and theoretical M-series XRPCSs, four sets of theoretical val-
the shift of atomic-level energies and hence alters the correspond- ues, σMtot (EM), σMtot (DM), σMtot (ED), and σMtot (DD), have been
ing transition energies. As a result of this, some of the non-radiative evaluated, as explained in Sec. 2. The first two sets of theoretical
transitions may even become energetically disallowed/allowed. Mul- cross sections {σMtot (EM), σMtot (DM)}, respectively, have been cal-
tiple vacancies also result in the availability of reduced num- culated using two sets of proton ionization cross sections based on
ber of electrons for certain radiative transitions, thereby directly the ECUSAR model37,38 and the DHS model;35,36 the fluorescence
impacting the corresponding fluorescence yields. The ab initio and CK/SCK yields are tabulated by McGuire.47 The latter two sets
theoretical calculations of different physical parameters incorporat- of values, {(σMtot (ED), σMtot (DD)}, respectively, have been calcu-
ing the multiple ionization effects and the many-body effects to the lated using two sets of proton ionization cross sections based on the
IPA models are quite complex. These multiple ionization effects ECUSAR model37,38 and the DHS model;35,36 the fluorescence and
have been included by statistical scaling58 based on specific charged CK/SCK yields are based on the DHS model.48,49 It has been found
particle induced Li (i = 1–3) sub-shell ionization probabilities to that the σMtot (EM) and σMtot (ED) values differ by up to 7% because
obtain the values of different physical parameters from their corre- of the differences in two sets of fluorescence and CK/SCK yields
sponding single vacancy state values available in the literature. How- based on the DHS model48,49 and those tabulated by McGuire47 used
ever, to the best of our knowledge, the use of such scaling to obtain to calculate these cross sections. Similarly, σMtot (DM) and σMtot (DD)
the Mi (i = 1–5) sub-shell physical parameters is not available in the values differ by up to 7%. Furthermore, σMtot (EM) and σMtot (DM)
literature. values for Au are found to differ by ∼2 to 25%. These differences in
two sets of XRPCSs are due to differences in two sets of theoretical
proton ionization cross sections, which, in turn, have arisen due to
3. Tabulated Experimental XRPCSs the use of different wave functions used in the ECUSAR39–42 and the
DHS35,36 model calculations.
3.1. Proton induced M-series XRPCSs
The experimental total M-series XRPCSs for
A thorough literature search yielded 25 papers pertaining Au3,4,6,7,9,10,18,19,21,22,24,25,27 available in the literature have been
to measurements of the experimental M-series XRPCSs for ele- compared with different sets of theoretical values in Figs. 7(a) and
ments La, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Hf, 7(b). It may be recalled that the DHS model35,36 based ionization
Ta, W, Re, Os, Ir, Pt, Au, Tl, Pb, Bi, Th, and U induced by cross sections are available only for proton energies up to 2.0 MeV;
0.05–39.34 MeV protons. The XRPCS values reported in the avail- therefore, above this energy, the comparison of experimental values
able publications3–10,18–27 are listed in Table 2. Different authors could be done only with two sets of calculated cross sections,
have quoted the uncertainties ∼3% to 34% in the measured M- σMtot (EM) and σMtot (ED). It is clear from Fig. 7(a) that the measured
series XRPCS values. Most of the reported measurements were per- σMtot (exp) values for incident proton energies ranging 0.3–39.3 MeV
formed using targets of thickness ∼2.7 to 50 μg/cm2 deposited on are found to differ from the σMtot (ED) and σMtot (DD) values, on
the 5–30 μg/cm2 thick carbon foil backing. However, in some cases, an average, by up to 34% and 24%, respectively, whereas these
Mylar,3,6 Kapton,7 Al foil,13,21 and organic substrate8 were also used differences increased enormously up to a factor ∼3.9 and ∼2.5,
as backing materials. On the other hand, some authors3,7,8,13,20,27 respectively, with incident proton energies decreasing from 0.3
performed these measurements using targets of thickness rang- to 0.05 MeV. Similar differences have been observed between
ing ∼173 to 654 μg/cm2 . The x-ray detector efficiency, in some the measured and two sets of theoretical values, σMtot (EM) and
reports,4,5,10,14,21,23 was determined by bombarding thin targets of σMtot (DM) [Fig. 7(b)].
low-Z elements with 1.5–2.0 MeV He ions. The resulting K-shell
x-ray yield was normalized to the Rutherford back scattered-particle 3.2. Helium ion induced M-series XRPCSs
yield, which was collected simultaneously along with the charac- The experimental M-series XRPCSs for impact of
teristic x rays. In some reports,7,9–11,13,16,17,22,24–27 the x-ray detec- 0.20–6.0 MeV 4 He ions on La, Pr, Nd, Sm, Eu, Gd, Dy, Ho,
tor efficiency was measured by using radioisotopes of 57 Co, 241 Am, Er, Yb, Lu, Hf, Ta, W, Re, Os, Ir, Pt, Au, Pb, Bi, Th, and U were
56
Fe, 153 Ba, and 152 Eu and in some cases10,11,16,17 using both the pro- reported in ten publications,4,5,10,13,15,23,28,29,31,32 whereas three
tons and helium ions, employing the “reference” K-shell ionization reports10,15,30 pertain to the measurements of these cross sections for
cross sections.59 In 17 publications, the measured data have been impact of 0.30–3.0 MeV 3 He ions on Ta, W, Re, Os, Au, Bi, and Th
presented in tabular form, whereas in the remaining eight papers, and two publications10,15 reported the simultaneous measurements
the measured values have been presented only graphically. These of the 3 He and 4 He ions induced M-series XRPCSs for Ta, W, Re,
cross sections11–17 presented graphically could not be included in Os, Ir, Pt, Au, Bi, and Th. All these reported experimental cross
Table 2. However, these publications have been included in the list of sections for 4 He and 3 He ion impact on different elements are listed
references. in Tables 3 and 4, respectively. The experimental cross sections
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TABLE 2. Proton induced total and line resolved experimental M-series XRPCSs (barns) for different elements with 59 ≤ Z
≤ 92 reported by different authors3–10,18–27
59 Pr
60 Nd
62 Sm
63 Eu
64 Gd
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TABLE 2. (Continued.)
65 Tb
66 Dy
67 Ho
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TABLE 2. (Continued.)
68 Er
69 Tm
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TABLE 2. (Continued.)
70 Yb
71 Lu
72 Hf
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TABLE 2. (Continued.)
73 Ta
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TABLE 2. (Continued.)
74 W
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TABLE 2. (Continued.)
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TABLE 2. (Continued.)
75 Re
76 Os
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TABLE 2. (Continued.)
77 Ir
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TABLE 2. (Continued.)
78 Pt
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TABLE 2. (Continued.)
79 Au
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TABLE 2. (Continued.)
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TABLE 2. (Continued.)
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TABLE 2. (Continued.)
81 Tl
82 Pb
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TABLE 2. (Continued.)
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TABLE 2. (Continued.)
83 Bi
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TABLE 2. (Continued.)
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TABLE 2. (Continued.)
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TABLE 2. (Continued.)
90 Th
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TABLE 2. (Continued.)
92 U
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TABLE 2. (Continued.)
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TABLE 3. 4 He ions induced total and line resolved experimental M-series XRPCSs (barns) for different elements with
59 ≤ Z ≤ 92 reported by different authors4,5,10,23,28,29,32
59 Pr
60 Nd
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TABLE 3. (Continued.)
68 Er
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TABLE 3. (Continued.)
71 Lu
72 Hf
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TABLE 3. (Continued.)
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TABLE 3. (Continued.)
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TABLE 3. (Continued.)
77 Ir
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TABLE 3. (Continued.)
78 Pt
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TABLE 3. (Continued.)
79 Au
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TABLE 3. (Continued.)
82 Pb
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TABLE 3. (Continued.)
83 Bi
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TABLE 3. (Continued.)
90 Th
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TABLE 3. (Continued.)
92 U
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TABLE 3. (Continued.)
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TABLE 4. 3 He ions induced total and line resolved experimental M-series XRPCSs (barns) for different elements with
73 ≤ Z ≤ 90 reported by different authors10,30
73 Ta
74 W
75 Re
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TABLE 4. (Continued.)
76 Os
79 Au
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TABLE 4. (Continued.)
83 Bi
90 Th
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TABLE 4. (Continued.)
plotting these cross sections as a function of a dimensionless scaling electron for specific element; n and me , respectively, represent the
parameter,61 which can be defined as principle quantum number of M-shell and the mass of electron, R is
the Rydberg constant; and Z2M is the average screened target atomic
ξM = 2vp /v2M θM , (6) number. The average M-shell binding energy (EM ) for a specific
element can be determined using the following relation:
where vp denotes the projectile ion velocity, θM (= n2 EM /Z2M
2
R)
is the reduced M-shell electron binding energy, and
(EM1 + EM2 + 2(EM3 + EM4 ) + 3EM5 )
v2M (= 2EM /me )1/2 corresponds to the velocity of the M-shell EM = , (7)
9
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FIG. 10. Proton induced experimental total M-series XRPCSs for different ele-
ments Z = 59–92 reported by different authors (Table 2) as a function of scal-
ing parameter defined as ξM = 2vp /v2M θM , where vp denotes the projectile ion
velocity, θM (= n2 EM /Z2M
2
R) is the reduced M-shell electron binding energy, and
v2M (= 2EM /me )1/2 corresponds to the velocity of the M-shell electron for specific
element. The black curve represents the least-squares fitted values, whereas the
magenta, red, and blue curves, respectively, denote present calculated theoretical
total M-series XRPCSs calculated using the PWBA model,34 ECUSAR model,37,38
and DHS model35,36 based proton ionization cross sections.
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ECUSAR model,37,38 and the DHS model35,36 based proton ioniza- This universal character has been used to parameterize the tabu-
tion cross sections have also been plotted as a function of the scaling lated experimental total M-series XRPCSs in terms of polynomials
parameter in Fig. 10. It is obvious from this figure that the exper- defined by Eq. (8). The proton and helium ion induced M-series
imental total M-series XRPCSs for different elements exhibited a XRPCSs for different elements deduced from the fitting coefficients
universal scaling similar to that shown by the theoretical total M- are recommended for use in different applications.
series XRPCSs. It may be noted that the experimental cross sections
show large variation between the minimum and maximum values Data Availability
for different elements over a wide range of proton energies consid-
ered in the present work; therefore, these were least-squares fitted to The data that support the findings of this study are available
polynomials in [log(ξM )] of the form from the corresponding author upon reasonable request.
X n References
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