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Year : 2012  |  Volume : 35  |  Issue : 3  |  Page : 111-125  

Overview of experimental works on secondary particle production and transport by high-energy particle beams

Emeritus of Tohoku University, Shimo-Shakujii, 6-43-5, Nerima-Ku, Tokyo, 177-0042, Japan

Date of Web Publication5-Sep-2013

Correspondence Address:
Takashi Nakamura
Emeritus of Tohoku University, Shimo-Shakujii, 6-43-5, Nerima-Ku, Tokyo, 177-0042
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Source of Support: None, Conflict of Interest: None

DOI: 10.4103/0972-0464.117665

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This overview gives a brief summary on the experimental results on three topics: (1) Thick target neutron yields produced by protons, deuterons, He and heavier ions having wide energy range from MeV to GeV, (2) spallation products production data together with induced activities by proton to U ion and (3) benchmark experiments on neutron shielding using various accelerators of MeV to GeV energies. These three items are essentially important for radiation safety of accelerator facility.

Keywords: Attenuation length, deuteron, heavy ion, neutron shielding, proton, spallation products, thick target neutron yield

How to cite this article:
Nakamura T. Overview of experimental works on secondary particle production and transport by high-energy particle beams. Radiat Prot Environ 2012;35:111-25

How to cite this URL:
Nakamura T. Overview of experimental works on secondary particle production and transport by high-energy particle beams. Radiat Prot Environ [serial online] 2012 [cited 2023 Mar 31];35:111-25. Available from: https://www.rpe.org.in/text.asp?2012/35/3/111/117665

  Introduction Top

Thick target neutron yield (TTY) generally means the angular-energy distribution of secondary neutrons produced from a thick target, which has enough thickness to fully stop the incident particles. The TTY data are indispensable for estimating source terms used in the accelerator shielding design. A number of experiments to give the TTY data have ever been published. Although it is difficult to survey all papers on TTY, the TTY papers up to 2000 have been collected in the Japanese book written by Nakamura [1] and the TTY data for projectile ions heavier than He ions of energies above about 100 MeV/nucleon have been published as the handbook written by Nakamura and Heilbronn. [2] Recently, the TTY data up to 2009 for light projectiles, mainly protons and deuterons have been summarized by Nakamura, [3] together with the TTY data for heavier projectiles of energies below about 100 MeV/nucleon.

In addition to TTY data, spallation products production cross section data up to 2010 are summarized together with excitation functions, mass-yield distributions and induced activities for various projectiles from proton to U ion. They are the basic data for induced activity estimation in high energy accelerator facilities. A systematic study has been performed by Michel et al., for protons [4] and for heavy ions from He to Ar ions, a comprehensive work has been carried out by a Japanese group and an American group using Heavy Ion Medical Accelerator in Chiba (HIMAC), National Institute of Radiological Sciences, Japan. These results are also cited in the handbook. [3]

Many experiments on neutron shielding have ever been performed using various accelerators. [5],[6] Among them, the benchmark experiments are defined here as follows:

  1. Neutron energy spectra penetrated through shields with different thicknesses are given.
  2. Source neutron energy spectrum is also given by experiment and/or calculation.
  3. Experimental geometry is relatively simple or well-defined.
These benchmark experiments are quite useful for investigating the accuracies of calculation codes and nuclear reaction model and cross section data, but they are still limited in number. The benchmark experiments are classified into two categories, one uses quasi-monoenergetic neutron source produced from the 7 Li (p, n) reaction and another uses continuous energy (white) neutron source produced from thick (stopping length) target by bombarding accelerated ions. Various neutron detectors have been used for the shielding experiments, such as organic liquid scintillator, spallation detectors of C, Al, Bi etc., self-TOF (Time-Of-Flight) detector, multi-moderator detector (Bonner ball).

  Thick Target Neutron Yield Top

TTY by protons

TTY by protons is summarized in [Table 1]. Many experimental results for various targets from Li to U are obtained for proton energy of 15 MeV up to 1.6 GeV at various accelerator facilities. The neutron detectors are mostly NE-213 organic liquid scintillator coupled with the TOF method and some with the unfolding technique. Activation detectors are also used in a few experiments. Typical experimental results are cited here for three proton energy regions of several tens MeV, a few hundreds MeV and above 500 MeV.
Table 1: General information on thick - target neutron yield experiments by proton beams

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[Figure 1] gives the neutron spectra at 0-150° in Cu target bombarded by 22, 30 and 40 MeV protons by Amos et al. [9] All spectra have two components; one below about 10 MeV especially for heavier target corresponds to neutrons produced almost isotropically through the equilibrium/evaporation process from a compound nucleus having a nuclear temperature of 1-2 MeV; the other above 10 MeV corresponds to neutrons, having forward-peaked at higher energies, produced by the pre-equilibrium and direct reaction (usually in cascade) processes. The neutron spectra become softer at large emission angle for heavier target where the evaporation process through a larger number of target nucleons is prominent. The neutron spectra therefore become harder for lighter target like carbon. This implies that lighter target nuclei are excited in a state of higher nuclear temperature.
Figure 1: Neutron yield spectra from stopping Cu target bombarded by protons at energies of 22, 30 and 40 MeV. Each energy group has spectra at 0, 30, 60, 90, 120 and 150°. Between the spectra labeled 0 and 150° are the other four spectra in monotonically descending order[9]

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[Figure 2] gives the neutron energy spectra at 15-150° in Pb target by 0.5 and 1.5 GeV protons by Meigo et al. [26] The neutron spectra have also two components, evaporation component below 10 MeV and pre-equilibrium/cascade component above 10 MeV, but the ratio between these two components is quite prominent. The ratio between evaporation and pre-equilibrium/cascade neutrons is almost equal for Fe especially at forward angles and the fraction of evaporation neutrons is much higher for Pb which has much larger numbers of nucleons. The measured spectra are compared with the NMTC/JAERI [34] and MCNP-4A [35] in [Figure 2] using free nucleon-nucleon cross section (NNCS) and in-medium NNCS. [36] In general speaking, the agreement between experiment and calculation is good within a factor of 2.
Figure 2: Neutron spectra for (a) 0.5 GeV and (b) 1.5 GeV protons incidence on thick lead target. Symbolds stand for the experimental results. Dash and solid lines show results calculated with NMTC/JAERI and MCNP-4A using free nucleon-nucleon cross section and in-medium NNCS, respectively[26]

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TTY by deuterons

TTY by deuterons is summarized in [Table 2]. Many experimental results for various targets from Li to U are obtained for deuteron energy of 8 MeV up to 200 MeV at various accelerator facilities, but mostly for the Be target by 15-50 MeV deuteron bombardment.
Table 2: General information on thick - target neutron yield experiments by deuteron beams

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The neutron energy spectrum based on the stripping reaction can be simulated on the basis of the Serber model, [46] an elegantly simple semi-classical theory for deuteron stripping. The generalization of the Serber model is given by effecting averages over the target thickness and emission angles by Menard et al. [38] The simulated results are compared with the measured results as shown for Be target bombarded by 50 MeV deuterons in [Figure 3]. [37] In the figure, the right flanks of the spectra above 25 MeV for 50 MeV deuterons are well reproduced by the Serber model. The neutron peak energies and production yields given by the model are lower than the experimental results. This behavior is due to the fact that the evaporated neutrons are considered to be emerging also from the stripping and direct nuclear collisions. The shape of the theoretical distribution exhibits a maximum at energy of neutrons lower than that given by the experiment by approximately 2 MeV.
Figure 3: (a) Experimental energetic distributions of neutrons for 50 MeV 2H incident energy on a thick Be target from Ref.[37]: filled circles at 0°, filled triangles with up-point at 5°, filled squares at 10° and filled triangles with down-point at 25 deg. These distributions are compared with theoretical ones: (a) 0, (b) 5, (c) 10 and (d) 25°. The dotted lines are to guide the eye

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TTY by He and heavier ions of energies lower than 100 MeV/nucleon

TTY by He and heavier ions of energies lower than 100 MeV/nucleon are summarized in [Table 3]. Projectiles are 3 He, 4 He(α), 6 Li, 7 Li, 11 B, 12 C and Ar of total energies from 40 MeV to 460 MeV and targets are from Be to Pb.
Table 3: General information on thick - target neutron yield experiments by He and heavier ion beams having lower than 100 MeV/nucleon energies

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Among of many experimental results on TTY by 4 He(α) and heavier projectiles, the Ta target results with 50 MeV 4 He(α) ions by Sarkar et al., [48] are shown in [Figure 4]. In [Figure 4], the spectra also have two components of evaporation and pre-equilibrium/cascade processes and the latter component decreases with increasing angles. The measured spectra are compared with the calculated spectra with the exciton model formalism [53] including the statistical multistep direct and the statistical multistep compound processes. The agreement between experiment and calculation is poor at 0° but becomes better at a large angle.
Figure 4: Neutron spectra from 181Ta target with 50 MeV alpha at 0, 30 and 60° emission angles. Experimental data are plotted in solid circles with error bars and the solid lines are the theoretical calculations of the extended exciton model[4]

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TTY by He and heavier ions of energies higher than 100 MeV/nucleon

[Table 4] contains a list of the secondary neutron thick-target data sets by He and heavier ions of energies higher than 100 MeV/nucleon. Unless otherwise noted, all targets are thick enough to stop the primary beam. The first column contains the beam ion species and beam energy in MeV/nucleon. The second column lists the targets used with each beam. The third column lists the spectra that were measured. TTY indicates that double-differential TTY were measured, n/dΩ indicate that angular and energy distributions were measured, respectively, and "total" indicates that total neutron yields were extracted. The total yields were usually limited to the angular range used in the measurements, so in most cases the total yields were not strictly "total" in the sense that they cover the distribution over all 4π steradians. The fourth column indicates the laboratory angles where spectra were measured. The fifth column lists the minimum neutron energy range measured. The last column indicates the accelerator facility where the measurements took place.
Table 4: General information on thick - target neutron yield experiments by heavy ions having higher than 100 MeV/nucleon energies[2]

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The double-differential TTY in the forward direction of 0-90° from the HIMAC series of experiments are shown in [Figure 5] for 400 MeV/nucleon C ions as an example, by Satoh et al., [56] which have reevaluated the former HIMAC experiments by Kurosawa et al., [54],[55],[59],[62] by changing the neutron detection efficiency calculation to a new code, SCINFUL-QMD [64] from the CECIL code. [65] In general, the spectra in the forward direction have a broad peak at the high-energy end. The peak energy usually occurs at about 60-70% of the beam energy per nucleon. As the target mass becomes lighter and the projectile mass increases, the high-energy peak becomes more prominent. Most of neutrons in this high-energy, forward region come from the breakup of the projectile and direct knock-on processes. The peak yield of the knock-on neutrons increases with a decrease in the mass number of target nuclei. This is because the ratio of the cross section of peripheral collision, which is a main source of the knock-on neutrons, to that of the central collision, which is a main source of the evaporation process, is inversely proportional to the radius of the target nucleus.
Figure 5: Neutron energy spectra for 400 MeV/nucleon C ion bombardment on thick Cu and Pb targets. Marks indicate the experimental data and solid lines indicate the PHITS calculation[56]

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At the high-energy end of the neutron spectra in the most forward direction, the high-energy tail spreads up to 2.5 times the incoming beam energy per nucleon, i.e., about 1000 MeV for 400 MeV/nucleon. This can be explained by considering high-momentum components of a Fermi motion in a nucleus. The projectile nuclei are highly excited through the direct collision with some nucleons moving in the target nucleus to produce the projectile-like fragments. The high energy neutrons are produced from the thus-excited projectile-like fragments. At energies below 20 MeV, the spectra are dominated by the breakup of the target, evaporation process. Because the target remnant is moving slowly in the laboratory frame, that source of neutrons is essentially isotropic. As such, target-like neutrons can be seen at all angles. As target mass increases, the relative contribution to the overall spectra from target breakup increases. This feature can be seen by comparing 400 MeV/nucleon C + C and C + Pb spectra at low energies.

As can be seen in [Figure 5], PHITS (Particle and Heavy Ion Transport code System) calculation [66] gives overall good agreement with the experimental data within a factor of three, except for a few cases. It is noted that the dropping curve at the high energy end of neutron spectra in the most forward direction is reproduced well by PHITS. A systematic underestimation however, appears around the broad peak of knock-on neutrons. This deviation should be further revised by considering the nucleon-nucleon interaction.

  Spallation Products Production Cross Section Data Top

An important component in the design of heavy-ion accelerator facilities is an accurate estimation of the radioactivities induced by spallation products in accelerator components and in shielding materials. For this purpose, the production cross sections for various spallation products have been measured from heavy-ion reactions by several groups. [Table 5] shows the various beams, targets and facilities used in the experiments, along with the relevant references.
Table 5: Listing of the beams, energies (MeV/nucleon), targets and facilities used to measure spallation product cross sections and/or induced activities.[2] The appropriate reference (s) for each entry is also listed

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Mass-yield distributions

The data can be summed over the same mass numbers to produce mass-yield (isobaric-yield) distributions. [Figure 6] shows the mass-yield distributions (in mb) for the 400- and 800-MeV/nucleon Ne, C and Si ions interacting in a Cu target, as examples by Yashima et al., at HIMAC. [74],[75] In general as the mass of the beam increases, the yield also increases. In the figure, produced nuclides can be divided into the following three groups; (I) target fragmentation induced from a reaction of which the impact parameter is small or projectile fragmentation for heavy projectile, (III) target fragmentation induced from a reaction of which the impact parameter is almost equal to the sum of projectile radius and target radius, (II) target fragmentation induced from a reaction of which impact parameter is in the medium of (I) and (III). The mass yields are somewhat independent of energy, although there appears to be a slight decrease in yield with increasing energy for the higher mass yields. [Figure 6] also gives the comparison between the experimental results and the PHITS calculations. The C/E (calculation/experiment) ratios are shown in [Figure 6]f. As shown in [Figure 6]f, the PHITS calculations in general agree well with the experimental values within a factor of 2 except for several products. The PHITS calculation gives a large underestimation of the cross sections, especially for the heavy-mass products.
Figure 6: Comparison of measured cross sections of radioactive nuclides produced in Cu for various projectiles with the PHITS Monte Carlo calculation.[75]

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Induced activities

The spatial distributions of residual activities of isotopes produced in thick copper target by bombarding various ion beams are also measured. [Figure 7]a-f show the spatial distributions of residual activities of 38 Cl, 49 Cr, 56 Mn and 61 Cu isotopes produced in Cu target as a function of Cu depth in the unit of beam range for p, He, C, Ne, Si, Ar ion beams with different energies at HIMAC. [76] The feature of these figures can be summarized as follows. When the mass number difference between Cu and the produced nuclide is large, nuclides are produced dominantly by the primary projectile reaction. The reaction cross sections therefore almost or slowly decrease with the target depth, according to the attenuation of projectile flux through the target. When the mass number difference between Cu and the produced nuclide is small, fraction of nuclides produced by secondary particles is large. With increasing mass number and projectile energy, the reaction cross section increases with the depth of Cu target due to the increasing contribution of secondary particle reactions. In [Figure 7], residual activity steeply increases near the projectile range in some cases. This is attributed to the projectile fragmentation just before stopping at the range. Since a projectile fragment has the same velocity and direction as the projectile ion, the projectile fragment stops at a slightly deeper point than the projectile range.
Figure 7: Spatial distribution of residual activities within Cu target depth. For example, "Ne[230]" signifies 230 MeV/nucleon Ne irradiation[76]

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  Benchmark Experiments on Neutron Shielding Top

Among of many experiments on neutron shielding using various accelerators, the benchmark experiments defined in the introduction are briefly described here. Two types of shielding benchmark experiments have ever been performed using the quasi-monoenergetic neutrons produced from the 7 Li (p, n) reaction and the continuous energy neutron sources.

Shielding experiments using quasi-monoenergetic neutron source

The experiments were performed at the following three cyclotron facilities,

  1. Experiments using 25 and 35 MeV p-Li neutrons at Cyclotron and Radioisotope Center (CYRIC), Tohoku University [83]
  2. Experiments using 43 and 68 MeV p-Li neutrons at Takasaki Institute for Advanced Radiation Application (TIARA), Japan Atomic Energy Agency [84],[85],[86]
  3. Experiments using 140, 246 and 352 MeV p-Li neutrons at Research Center for Nuclear Physics (RCNP), Osaka University. [87],[88],[89]
The physical properties of neutron sources, shielding materials and neutron detectors of these three experiments are summarized in [Table 6] and here in this paper, only RCNP experiments are briefly described.
Table 6: Physical properties of neutron sources, shielding materials and neutron detectors for p-Li quasi-monoenergetic neutron source

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Proton beams extracted from the cyclotron were transported to the experimental hall and impinged onto a 10 mm thick Li target placed in a vacuum chamber. Protons passing through the target were swept out towards the beam dump by the swinger magnet to measure the proton beam intensity with a Faraday cup. The proton beam intensity was also monitored with a plastic scintillator by scattering through a thin plastic film. Neutrons produced at 0° from the Li target were extracted into the TOF room of 100 m length through a concrete collimator of 10 cm × 12 cm aperture and 150 cm thickness while charged particles were rejected by a vertical bending magnet located in the collimator. The neutrons extracted into the TOF room were measured by a 12.7-cm diam × 12.7-cm long NE213 scintillator with the TOF method, as shown in [Figure 8]. The energy spectra converted from the TOF spectra for 90, 140, 246, 352 and 389 MeV proton energies are shown in [Figure 9]. [87] A sharp monoenergetic peak can clearly be seen.
Figure 8: Experimental setup for shielding experiment at Research Center for Nuclear Physics[88,89]

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Figure 9: Energy spectra of source neutrons generated by 7Li (p, n) reaction using 140, 250, 350, 392 MeV protons obtained with the TOF method[87]

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The shielding experiment was performed with 140, 246 and 352 MeV p-Li quasi-monoenergetic neutrons. [87],[88] Concrete and iron shield blocks of 120 cm × 120 cm sizes having 10 cm and 5 cm thickness, respectively were laminated to change the total thickness up to 2 m for concrete and 1 m for iron. They were fixed just after the concrete collimator. The NE213 scintillator and the Bonner ball with 3 He counter were set behind the shield to get the neutron energy spectra down to thermal energy. [Figure 10] gives the neutron energy spectra penetrated through iron and two kinds of concrete (low activation limestone concrete and ordinary concrete) for 140 MeV p-Li neutron source. The measured spectra are compared with the calculated results using three Monte Carlo transport codes, PHITS [66] and Monte Carlo N-Particle eXtended (MCNPX). [90] The agreement between experiment and calculation is in general good, but in the continuum energy region below the peak energy the calculation gives underestimation; although, the PHITS code gives better agreement with the measurement than other two codes.
Figure 10: Comparison of the neutron energy spectra transmitted through iron (upper left figure) and concrete shield (upper right figure) with various thicknesses for the 140 MeV p-7Li quasi-monoenergetic neutrons between the NE213 experiment and the Monte Carlo codes (PHITS and Monte Carlo N-Particle eXtended).[89]

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Shielding experiments using continuous energy neutron source

A number of shielding experiments have ever been done using the continuous energy neutron sources at medium to high energy accelerator facilities as listed in [Table 7], but here only one experiment using 800 MeV protons at the ISIS spallation neutron source facility, Rutherford Appleton Laboratory (RAL), UK is briefly described as an example. [100]
Table 7: Physical properties of neutron sources, shielding materials and neutron detectors for projectile energies above 100 MeV/nucleon[5]

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The shielding experiment was performed as an international collaborative work of Tohoku University, High Energy Accelerator Research Organization (KEK), Institute of Physical and Chemical Research (RIKEN) and RAL. The ISIS facility consists of a 70-MeV H-linear accelerator, an 800-MeV proton synchrotron and a spallation neutron target station. The beam intensity is about 170 μA at the target with 50-Hz repetition rate. A cross sectional view around the target station along the 800-MeV proton beam axis is shown in [Figure 11]. The tantalum target is assembled by the 90-mm diameter tantalum disk of various thicknesses from 8.2-mm to 26.7-mm and the gap between each disk for the cooling water (D 2 O) is 1.75-mm. This stopping-length tantalum target (total length of 296.5 mm) is placed at the center of the stainless-steel vessel. The moderators of heavy water and beryllium reflectors are placed around the target. The upward direction of the target station is shielded with a shielding plug of 284-cm thick steel and 97-cm thick ordinary concrete. This experiment was performed at the top of a shielding plug (shield top) just above the target station. As seen in [Figure 11]a, a big bent duct of about 42.5-cm × 42.5-cm cross section in which helium gas flows for filling the target vessel, reaches the shield top through the bulk shield downstream from the target. Neutrons that leaked from this duct became large background components in the measurement at the shield top. An iron-igloo (60-cm thick, 120-cm inner diameter and 196-cm high) was set on the top center of the target station to reduce the background neutrons and an additional shield of concrete or iron was piled up inside the igloo. In this shielding experiment, the additional shielding blocks of ordinary concrete and iron were placed upon the top center of the bulk shield just above the target as shown in [Figure 11]b. The additional concrete (20-120-cm thickness) and iron (10-60-cm thickness) blocks were assembled by 119-cm-diameter by 20-cm-thick blocks of 2.36-g/cm 3 density and by 119-cm-diameter by 10-cm-thick blocks of 7.8-g/cm 3 density, respectively. The concrete blocks contain the iron mesh for reinforcement. Since the neutrons were produced from the target as the burst pulses corresponding to 50-Hz synchrotron operation, the pulse counters could not be used because of the pulse pile-up problem and the activation detectors of C, Al, Bi and the gamma-ray insensitive type Bonner ball inserted In were then used. The attenuation lengths of concrete and iron for high-energy neutrons above 20 MeV produced at 90° to the proton beam were obtained from the 12 C (n, 2n) 11 C reaction rates of graphite.
Figure 11: Cross-sectional views of the neutron spallation target station with an 800-MeV proton beam at ISIS[100]

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The neutron spectra penetrated through concrete and iron were obtained from the reaction rates of the 12 C (n, 2n) 11 C, 27 Al (n, α) 24 Na, 209 Bi (n, xn) 210-x Bi (x = 4-10) and 115 In (n, γ) 116 m In in the energy range of thermal to 400 MeV. [Figure 12] shows the measured and calculated neutron energy spectra in lethargy unit on the shield top floor, behind the 60-cm-thick additional concrete and behind the 30-cm-thick additional iron at the shield top center. A calculation of neutron penetration through a thick shield was performed with a three-dimensional multi-layer technique using the MARS14 (02) Monte Carlo Code [102] to compare with the experimental shielding data. The calculated energy spectrum behind the additional concrete shield is in good agreement with the experiment within about 40% in the energy region above 1 MeV. Generally, the calculated energy spectra agree well with the measured ones within a factor of 2 over a broad energy range with the maximum differences reaching a factor of 3 except at thermal energy. This good agreement is marvelous because the neutron fluence and dose decrease about 10 -7 order of magnitude from the Ta target to the shield top.
Figure 12: Comparison between the calculated and measured neutron energy spectra on the shield top floor, behind the additional concrete (60 cm thick) and iron (30 cm thick) shields[100,101]

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Attenuation lengths of neutron dose equivalent

These experiments in [Table 6] and [Table 7] give the attenuation lengths of neutron ambient dose equivalent. For direct comparison of these results, the effective maximum value E max of the source neutron energy was estimated from measurements and calculations and the attenuation length was evaluated as a function of the effective maximum value. [Figure 13] shows the dose attenuation length λD as a function of E max . [5] The λD values for concrete keep an almost constant value of about 30 g/cm 2 up to several tens MeV and gradually increase above 100 MeV, then reach about 130 g/cm 2 beyond a few hundreds MeV. While for iron, the λD values slightly increase about 100 g/cm 2 at several tens MeV, but a big deviation about 210 g/cm 2 at HIMAC and 340 g/cm 2 at ISIS in several hundreds MeV region. This may be due to the experimental condition.
Figure 13: Comparison of attenuation lengths of neutron dose rates for concrete and iron as a function of the effective maximum energy of source neutrons[5]

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  Conclusion Top

This overview gives a brief summary on the experimental results up to 2010 on three topics: (1) TTY produced by protons, deuterons, He and heavier ions having wide energy range from MeV to GeV, (2) spallation products production data together with induced activities by proton to U ion and (3) benchmark experiments on neutron shielding using various accelerators of MeV to GeV energies. These data will be very useful both as benchmark data for computer code validation and as the source term data for accelerator shielding design calculation and induced activity evaluation.[110]

  References Top

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  [Figure 1], [Figure 2], [Figure 3], [Figure 4], [Figure 5], [Figure 6], [Figure 7], [Figure 8], [Figure 9], [Figure 10], [Figure 11], [Figure 12], [Figure 13]

  [Table 1], [Table 2], [Table 3], [Table 4], [Table 5], [Table 6], [Table 7]

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