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NIM B

Beam Interactions
with Materials & Atoms
Nuclear Instruments and Methods in Physics Research B 248 (2006) 1–6
www.elsevier.com/locate/nimb

Proton stopping power in a group of bioorganic compounds


over the energy range of 0.05–10 MeV
a,*
Zhenyu Tan , Yueyuan Xia b, Mingwen Zhao b, Xiangdong Liu b

a
School of Electrical Engineering, Shandong University, Jinan 250061, Shandong, PR China
b
Department of Physics, Shandong University, Jinan 250100, Shandong, PR China

Received 14 February 2006; received in revised form 19 April 2006


Available online 5 June 2006

Abstract

The systematic calculations of the stopping powers (SPs) for 0.05–10 MeV protons in a group of 10 important bioorganic compounds,
i.e. DNA, five bases, three fatty acids and cellulose, have been performed. The calculations are based on the dielectric model of Ashley
and on an evaluation of optical energy loss function (OELF) for the bioorganic compounds considered, most of which have no available
optical data. Higher-order corrections, Barkas-effect correction and Bloch correction, are included and a concise form of SP calculation
corresponding to Barkas-effect is presented by incorporating the evaluated OELF. Especially, the dependences of SP calculations on the
two choices of the minimum impact parameter a are analyzed in detail, and hence an appropriate parameter a is determined for organic
media. For the tested organic compounds the proton SPs calculated by use of the determined a are in excellent agreement with the tab-
ulated values based on experimental data. The presented data are the first results of the proton SPs for the 10 bioorganic compounds in
the energy range from 0.05 to 10 MeV, and might be useful for studies of various radiation effects in these materials.
Ó 2006 Elsevier B.V. All rights reserved.

PACS: 34.50.Bw; 61.82.Pv

Keywords: Stopping power; Dielectric theory; Bioorganic compounds; Radiation biology

1. Introduction eter, the mean excitation energy and additional theoretical


calculations for shell corrections. At the intermediate ener-
The stopping power (SP) of bioorganic materials for gies ranging from 50 keV to several hundreds of keV, the
proton is a subject of great importance in many fields of cases in the acquirement of proton stopping powers by
fundamental and application researches, such as radiation both theory and experiment are complex because of chang-
biology and radiotherapy. In particular, the use of protons ing mechanisms of proton–electron interactions. The
in radiotherapy offers a good potential to spare healthy tis- detailed reviews on this can be found elsewhere [6,7].
sues due to their characteristic depth dose curve [1,2], Another theoretical description for the interaction
where the knowledge of proton SP in biological tissues is between charged particle and medium is the dielectric
essential. In the high-energy range, i.e. proton energy E is response theory, which was first developed by Lindhard
larger than several hundreds of keV, the Bethe’s theory and Ritchie [8,9]. The SP calculation based on this theory
[3–5] can be used for the calculation of the SP for proton. need not know the mean excitation energy, and includes
However, this theory requires a material-dependent param- the shell corrections in a self-consistent way. In the frame
of the dielectric response theory, many works [10–14] have
*
Corresponding author. Tel.: +86 0531 88392806; fax: +86 0531
been done to evaluate the SPs of organic materials for low-
82955999. energy electrons. However, the reports on the SP calcula-
E-mail address: tzy@sdu.edu.cn (Z. Tan). tions for proton in organic compounds by utilizing the

0168-583X/$ - see front matter Ó 2006 Elsevier B.V. All rights reserved.
doi:10.1016/j.nimb.2006.04.073
2 Z. Tan et al. / Nucl. Instr. and Meth. in Phys. Res. B 248 (2006) 1–6

dielectric model are sparse. Ashley [15] developed an opti- obtained from experimental optical data. However, most
cal-data model to calculate the proton SP of the condensed of the bioorganic compounds under consideration have
matters including organic compound. Ashley’s approach no available optical data. The OELFs for these bioorganic
also took into account the higher-order corrections, i.e. compounds will be therefore evaluated using the approach
the Barkas-effect correction and the Bloch correction. By presented previously [14]. This approach may be outlined
extending Ashley’s model [15], Akkerman et al. [7] have as follows:
described a method to estimate the proton SP in 10 organic 8
< f1 ð
> hx; a; b; cÞ; hx 6 40 eV

compounds in the range of proton energies 50–500 keV. In
Im½1=eðxÞ ¼ f2 ð hx; y 0 ðaÞ; y 1 ; y 2 Þ; 40 eV 6 
hx 6 50 eV ;
Akkerman et al’s calculation, the dielectric theory was used >
:
for the calculations of the SP from valence electron excita- f3 ð
hxÞ; hx P 50 eV

tion, and Gryzinski’s binary encounter theory [16] was ð4Þ
employed for those from the core-electron ionization, thus
where f1(⁄x; a, b, c) is a single Drude-type function given
resulting in a seemingly fragmentary model. A common
by the formula
feature of these two works is that the numerical evaluation
of optical energy loss function (OELF) needs to make use aðhxÞ
f1 ðhx; a; b; cÞ ¼ ; ð5Þ
of experimental optical data. ½ðhxÞ  b2 2 þ c2 ðhxÞ2
2

In this work we report systematic calculations of SPs for


0.05–10 MeV protons in a group of 10 important bioorganic and the parameters b and c can be calculated by
compounds: DNA, five bases, three fatty acids and cellulose. b ¼ 19:927 þ 0:9807Z; ð6Þ
The calculations are based on Ashley’s model [15] and incor- c ¼ 13:741 þ 0:3215Z; ð7Þ
porate an evaluation approach [14] for OELF because most
of the bioorganic compounds considered have no available with Z, the mean atomic number of organic compounds;
optical data. The dependences of the SP calculations on f3(hx) can be obtained numerically by use of atomic photo-
the two choices of the minimum impact parameter a con- absorption data of Henke et al. [18] over the photon energy
cerned in the Barkas-effect correction are also analyzed in range of 50–30,000 eV; f2(hx); y0(a), y1, y2) is an parabolic
detail for organic media, and an empirical determination interpolation function with the parameters y0(a), y1 and y2,
of the parameter a is presented. The proton SPs calculated so as to link the f1 and f3 smoothly.
with the determined a for the tested organic compounds, In f2(hx; y0(a), y1, y2), the parameters y1 and y2 are
polyethylene, mylar, polystyrene, toluene and tissues-equiv- given by f3 at energies hx = 50 eV and 60 eV, respectively,
alent gas, are compared with the tabulated values [17]. and the parameter y0(a) is the value of f1 at energy
hx = 40 eV. Finally, the parameter a, and thus y0(a), is
2. Description of the method determined by the following f-sum rule due to dielectric
response theory:
Including the higher-order corrections, the stopping Z 1
2
power of a medium for a proton can be expressed as a Z¼ 2 2 ðhxÞIm½1=eðxÞdðhxÞ; ð8Þ
ph XP 0
sum of there terms, i.e.
where Xp = (4pne2/m)1/2, n = Navq/M is the density of mol-
dE
SP ¼ þ SP1 þ SP2 ; ð1Þ ecule, Nav is Avogadro’s number, q is the bulk density and
dS M is the molecule weight, Z is the total numbers of elec-
where dE/dS is basic stopping power, SP1 and SP2 corre- trons per molecule and m is the mass of electron.
spond to the Barkas-effect correction and the Bloch correc- As pointed out in previous work [14], there are only 14
tion, respectively. organic compounds for which the experimental optical
According to Ashley [15], the basic stopping power can data, i.e. the refractive index and the extinction coefficients,
be written as are available at photon energies below a few tens of eV.
dE 1 These 14 organic compounds were listed in work of
¼ 0:6015 0 Tanuma et al. [12]. For these 14 organic compounds, the
dS E
Z E0 OELFs evaluated by Eq. (4) are generally in good agree-
 ðhxÞIm½1=eðxÞvðaÞdð
hxÞ ðeV=ÅÞ; ð2Þ ment with those obtained using the experimental optical
0 data. As an example, the OELFs of guanine (C5H5N5O)
where E (in eV) is the kinetic energy of proton, E 0 = calculated by using Eq. (4) and experimental optical data
E/1837, hx (in eV) is the energy transfer, Im[1/e(x)] is [19], respectively, are displayed in Fig. 1 for the purpose
the optical energy loss function (OELF) and v(a) is of the comparison. It is clear that the OELF evaluated
by empirical approach due to Eq. (4) agrees well with that
vðaÞ ¼ ln½ð1  a þ sÞ=a; ð3Þ
pffiffiffiffiffiffiffiffiffiffiffiffiffiffi from the experimental optical data, especially at energies
0
hx/2E and s ¼ 1  2a.
with a =  larger than 10 eV. It is also observed from Fig. 1 that for
As shown in Eq. (2), the calculations of SP require deriv- the OELF from the experimental optical data a weaker
ing the OELF. In general, the numerical OELF can be peak appears at 6 eV, which is omitted in the empirical
Z. Tan et al. / Nucl. Instr. and Meth. in Phys. Res. B 248 (2006) 1–6 3

1.6 Extending Ashley’s approach and includingpffiffiffiffiffiffi the higher-


order corrections with the use of a ¼ 3:688=  hx, Akker-
man et al. [7] has calculated the SPs of polyethylene for
1.2 Guanine proton in the energy range of E 6 500 keV. At the energies
of E 6 300 keV Akkerman et al.’s calculations give the
SPs smaller than the tabulated values [17]. Using the
Im [-1/ε(ω)]

0.8 scheme described in this work and choosing the two differ-
ent minimum impact parameters mentioned above, respec-
tively, we have calculated the proton SPs of polyethylene in
0.4
the energy range of E 6 10 MeV. The calculated SP as a
function of proton energy are presented in Fig. 2 whereas
the evaluations from Akkerman et al. [7] and the tabulated
values [17] are also displayed in this figure for comparison.
0.0
Similarly,pffiffiffiffiit is seen clearly that with the choice of a ¼
88:748= E the present calculations, compared to the tabu-
0 20 40 60 80 lated values, overestimate the SPs at the energies E 6
Photon energy (eV) 300
p ffiffiffiffiffiffi keV, the SPs calculated by adopting a ¼ 3:688=
Fig. 1. Comparison of the optical energy loss functions for guanine. (—) hx are consistent with those from Akkerman et al. [7],
evaluated from the empirical approach due to Eq. (4); (h) calculated from and both are smaller than the tabulated values in the
the experimental optical data [19]. regions of E 6 200 keV.
According to above calculations and comparisons, it is
approach. However, the influence of this very small differ- shown clearly that for organic compound and at the ener-
ence on the calculations of SP is ignorable. gies below 200 keV,pthe ffiffiffiffi proton SPs calculated with the
For the SP2 corresponding to the Bloch correction, it choice of a ¼ 88:748= E are considerably large and those
pffiffiffiffiffiffi
can be calculated from Eqs. (10) and (11) of [15]. obtained using a ¼ 3:688= hx are evidently small, when
In terms of the principles described in Ashley [15] for the compared with the tabulated values. This fact is of the
calculation of SP1, and especially utilizing above Eq. (8), enlighten significance, and thus motivate us to take a as
which the evaluated OELFs satisfy, the SP1 can be 88:748 3:688
a ¼ k1 pffiffiffiffi þ k2 pffiffiffiffiffiffi ; ð11Þ
expressed in a concise form E hx
1 where k1 and k2 are two weight coefficients to obey
SP1 ¼ 1:1079
ðE Þ 0 5=2 k1 + k2 = 1.
Z 4E0
From Eq. (11), it is clear that the two general choices for

2
ðhxÞ dð
hxÞIm½1=eðxÞIðnÞ ðeV=ÅÞ; ð9Þ a is two limit cases of Eq. (11), i.e. when k1 = 1 and k2 = 0,
0 a corresponds to the minimum impact parameter suggested
where n ¼ 5:811 phxffiffiE a, with a a minimum impact parameter
to be discussed later, I(n) is a tabulated function [20] and 16
this function may be approximated [15,21] by
8 14
>
> ð3p=2Þ lnð1=nÞ  2:417  2pn2 ½ðln nÞ2 polyethylene
>
< þ1:14 lnn  0:33n < 0:25 12
IðnÞ ¼ :
>
> ð0:5986 þ 0:9962=n  0:1233=n2 Þn3=4 0:25 6 n < 1
>
: 10
SP (eV/Å)

9:052 expð3:72n þ 0:217n2 Þ 1 6 n 6 2


8
ð10Þ
There are two choices for the minimum impact parame- 6
pffiffiffiffiffiffi
ter a. One is a ¼ 3:688=  hx suggested by Jackson
pffiffiffiffi and 4
McCarthy [22] and the other is a ¼ 88:748= E as given
by Lindhard [23]. Emphasizing aluminum as a test, Ashley 2
[15] has in detail analyzed the dependence of the proton SP
calculations p
onffiffiffiffi the two choices of a. It was shown that with 0
a ¼ 88:748= E the calculated SPs of aluminum agree rea- 102 103 104
sonably well with the experimental data. However, for Proton energy (keV)
organic material polystyrene and using the same choice
Fig. 2. Stopping power (SP) results as a function of proton energy for
for a, Ashley’s evaluations for the SPs are considerably polyethylene. (—) Calculated with a from Lindhard [23]; (    ) calculated
large at the energies lower than 200 keV when compared with a from Jackson and McCarthy [22]; (j) tabulated values [17]; (h)
with the tabulated values [24] based on experimental data. calculated by Akkerman et al. [7]; (—) calculated with empirical a.
4 Z. Tan et al. / Nucl. Instr. and Meth. in Phys. Res. B 248 (2006) 1–6

by Lindhard [23], and if k1 = 0 and k2 = 1, then a is that 50 keV. In Fig. 3(a), for mylar
pffiffiffiffi the SPs evaluated
pffiffiffiffiffiffi using
given by Jackson and McCarthy [22]. Therefore, the prob- the parameter a ¼ 88:748= E and 3:688= hx, respec-
ing calculations by taking different k1 and k2 under the tively, have also been given. Being similar to the cases
restriction of k1 + k2 = 1 have been done for polyethylene, pffiffiffiffi E < 200
pointed out above for polyethylene, at energies
and the calculated SPs are compared with the tabulated keV the stopping powers with a ¼ 88:748= E are obvi-
pffiffiffiffiffiffi
values [17]. We found empirically that the stopping powers ously large and those by use of a ¼ 3:688= hx are small,
evaluated with k1 = 0.6 and k2 = 0.4 are in close agree- compared with the tabulated values. It should be seen that
ment with the tabulated values except for those at energies at energies below 50 keV and with empirical parameter a,
below 50 keV, which is also shown in Fig. 2. In order to the deviation of the calculated SPs from the tabulated val-
further examine the reliability of proton SP calculations ues is still significantly large. Hence, as pointed out by
with the parameter a due to k1 = 0.6 and k2 = 0.4, we have Akkerman et al. [7], for these energies Lindhard’s SP the-
calculated the proton SPs of organic compounds, mylar, ory and its further improvements are preferable.
polystyrene, toluene and tissues-equivalent gas. These
organic materials are selected because their tabulated stop- 3. Proton stopping powers in a group of bioorganic
ping powers needed for comparison were available. In the compounds
energy range of E 6 10 MeV, the calculated SPs versus
proton energy for these compounds are plotted in Fig. 3 Based on above calculations and comparisons, we will
and compared with the tabulated values [17]. We can see adopt the empirical a value given by Eq. (11) with
that an excellent agreement between the SPs calculated k1 = 0.6 and k2 = 0.4 for the calculations of the proton
with empirical a and the tabulated values is obtained above SPs of 10 bioorganic compounds: DNA, adenine

12
16

14 10
(a) Mylar (c) Toluene

12
8
SP (eV/Å)

10
SP (eV/Å)

6
8

6 4

4
2
2

0 0

2 3 4 2 3 4
10 10 10 10 10 10
Proton energy (keV) Proton energy (keV)

14 0.014

12 0.012 (d) Tissue-equivalent gas


(b) Polystyrene
10 0.010
SP (eV/Å)

SP (eV/Å)

8 0.008

6 0.006

4 0.004

2 0.002

0 0.000
2 3 4 2 3 4
10 10 10 10 10 10
Proton energy (keV) Proton energy (keV)

Fig. 3. Stopping power (SP) results as a function of proton energy for (a) mylar, (b) polystyrene, (c) toluene and (d) tissue-equivalent gas. (– – –)
Calculated with a from Lindhard [23]; (  ) calculated with a from Jackson and McCarthy [22]; (j) tabulated values [17]; (—) calculated with empirical a.
Z. Tan et al. / Nucl. Instr. and Meth. in Phys. Res. B 248 (2006) 1–6 5

(C5H5N5), guanine (C5H5N5O), thymine (C5H6N2O2), several tens of eV [19,25,26]. We can therefore obtain the
cytosine (C4H5N3O), uracil (C4H4N2O2), oleic acid OELF for these three bioorganic compounds in the follow-
(C18H34O2), linoleic acid (C18H32O2), arachidonic acid ing manner: for energies below 50 eV, the numerical OELF
(C20H32O2), cellulose (C6H10O5). Table 1 presents mass is calculated from experimental optical data and for ener-
density q, molecule weight M and mean atomic number gies larger than 50 eV the OELF is derived from atomic
Z of theses 10 bioorganic compounds. According to the photoabsorption data of Henke et al. [18]. For the other
composition of the base of the sodium salt of calf thymus compounds lacking experimental optical data, the OELF
DNA [25], an equivalent unit of the DNA molecule has is evaluated from Eq. (4).
been constructed. This equivalent unit consist of 58% A– Applying Eq. (4), the evaluated OELFs satisfy the f-sum
T (adenine–thymine base pair) and 42% G–C (guanine– rule naturally. Usually, another check for the accuracy of
cytosine base pair). the approach to evaluate OELF is to calculate the mean
In the 10 bioorganic compounds considered, for only ionization potential I by using the OELF, i.e.
guanine, DNA and adenine were the experimental optical Z 1
2
data available in the range of photon energies lower than ln I ¼ 2
ðhxÞIm½1=eðxÞ lnðhxÞdðhxÞ: ð12Þ
pZðhXp Þ 0
From Eq. (12), the I values for these 10 bioorganic com-
Table 1
pounds have been calculated and listed in Table 1. In addi-
Material parameters and I values for 10 bioorganic compounds
tion, the corresponding I values expected by Bragg’s
Material q (g/cm3) M Z I (eV)
additive rule are also displayed in Table 1. It is clear that
Calculated Expected the calculated results show a good agreement with expected
DNA 1.35 662 5.185 86.64 90 data.
Adenine 1.35 135.14 4.667 73.90 71.4 According to the method described above and with the
Guanine 1.58 151.14 4.875 78.25 75
evaluated OELFs, the systematic calculations of the proton
Thymine 1.48 126.12 4.4 74.09 76.1
Cytosine 1.3 111.11 4.462 73.22 74.6 SPs for the 10 bioorganic compounds in the energy range
Uracil 1.32 112.09 4.833 76.77 79.2 from 0.05 to 10 MeV have been carried out. The calculated
Oleic acid 0.89 282.45 2.926 59.83 61.1 results are listed at selected energies in numerical form in
Linoleic acid 0.9 280.44 3 60.52 62 Table 2. In order to make this table compact and clear,
Arachidonic acid 0.92 304.46 3.111 61.50 63.2
we use the code number, from 1 to 10, to represent the
Cellulose 1.35 162.14 4.095 74.43 77.6
10 compounds, and these are shown in Table 2. From

Table 2
SPs (in unit eV/Å) with higher-order corrections for: 1 – DNA, 2 – Adenine, 3 – Guanine, 4 – Thymine, 5 – Cytosine, 6 – Uracle, 7 – Oleic acid, 8 – Linoleic
acid, 9 – Arachidonic acid, 10 – Cellulose
E (keV) 1 2 3 4 5 6 7 8 9 10
50 5.095 7.115 7.698 7.729 6.922 6.298 7.151 7.071 7.009 7.172
60 7.439 9.443 10.41 10.25 9.147 8.565 8.654 8.592 8.566 9.448
70 8.665 10.59 11.76 11.46 10.23 9.694 9.295 9.246 9.245 10.53
80 9.227 11.06 12.33 11.95 10.66 10.17 9.481 9.441 9.454 10.95
90 9.459 11.19 12.52 12.10 10.78 10.33 9.433 9.401 9.423 11.07
100 9.502 11.13 12.50 12.05 10.73 10.32 9.260 9.232 9.260 11.04
150 8.833 10.03 11.40 10.95 9.697 9.440 8.047 8.036 8.074 10.07
200 7.926 8.869 10.13 9.719 8.586 8.406 7.006 7.001 7.041 8.959
300 6.480 7.136 8.191 7.843 6.919 6.809 5.534 5.534 5.568 7.249
400 5.492 5.967 6.869 6.576 5.794 5.720 4.590 4.591 4.621 6.092
500 4.782 5.144 5.931 5.678 5.000 4.944 3.938 3.939 3.965 5.268
600 4.260 4.551 5.251 5.030 4.425 4.382 3.479 3.482 3.506 4.670
700 3.864 4.109 4.742 4.548 3.997 3.961 3.147 3.150 3.173 4.223
800 3.544 3.758 4.337 4.162 3.655 3.625 2.881 2.885 2.907 3.864
900 3.282 3.481 4.015 3.849 3.381 3.353 2.662 2.666 2.688 3.567
1000 3.061 3.250 3.747 3.587 3.153 3.125 2.478 2.482 2.503 3.317
1500 2.332 2.471 2.850 2.723 2.395 2.375 1.865 1.869 1.887 2.513
2000 1.905 2.013 2.325 2.219 1.951 1.938 1.511 1.515 1.529 2.048
3000 1.415 1.489 1.722 1.642 1.444 1.436 1.111 1.114 1.125 1.516
4000 1.137 1.194 1.381 1.317 1.157 1.152 0.887 0.889 0.899 1.216
5000 0.956 1.002 1.160 1.105 0.971 0.968 0.743 0.745 0.753 1.021
6000 0.829 0.867 1.003 0.956 0.840 0.838 0.641 0.643 0.650 0.883
7000 0.733 0.767 0.887 0.845 0.742 0.740 0.566 0.568 0.574 0.781
8000 0.659 0.687 0.796 0.759 0.666 0.665 0.507 0.509 0.515 0.701
9000 0.599 0.624 0.723 0.689 0.605 0.604 0.461 0.462 0.467 0.637
10,000 0.550 0.573 0.664 0.632 0.555 0.554 0.422 0.424 0.428 0.584
6 Z. Tan et al. / Nucl. Instr. and Meth. in Phys. Res. B 248 (2006) 1–6

10 bioorganic compounds have been performed. The calcu-


lations include the higher-order corrections, and the
choices of the minimum impact parameter a, concerned
10 in the Barkas-effect correction, are analyzed in detail for
organic media. On the basis of this, an empirical determi-
nation of the parameter a is presented, which is important
SP (eV/Å)

for the calculations of the proton SPs in organic com-


DNA
Adenine
pounds. The calculated proton SPs for the 10 bioorganic
Guanine compounds in the energy range of 0.05–10 MeV are pre-
1 Thymine sented here for the first time, and can be used for studies
Cytosine of various radiation effects in these materials.
Uracil

Acknowledgements
2 3 4
10 10 10 This work was supported by the Foundation of Ministry
Proton energy (keV) of Education of China under Grant No. 20050422038 and
Fig. 4. Stopping power (SP) results as a function of proton energy for by the Natural Science Foundation of Shandong Province
DNA and the five bases. of China under Grant No. Y2005D02.

the calculated results, as a group these bioorganic com-


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[22] J.D. Jackson, R.L. McCarthy, Phys. Rev. B 6 (1972) 4131.
4. Summary [23] J. Lindhard, Nucl. Instr. and Meth. B 2 (1976) 1.
[24] J.F. Janni, At. Data Nucl. Data Tables 27 (1982) 147.
[25] T. Inagaki, R.N. Hamm, E.T. Arakawa, L.R. Painter, J. Chem. Phys.
Based on the optical-data model of Ashley [15] and on 61 (1974) 4246.
the evaluation approach of OELF [14], the systematic cal- [26] E.T. Arakawa, L.C. Emerson, S.I. Juan, J.C. Ashley, M.W. Williams,
culations of the SPs for 0.05–10 MeV protons in a group of Photonchem. Photobiol. 44 (1986) 349.

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