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Introduction During the fission process the 235U nucleus first absorbs a neutron, and a 236U compound nucleus is formed in an excited state. This is unstable, and fission into two medium-sized fission fragments1[1]. Additionally, a few neutrons are also emitted (for the 235U the average number of emitted neutrons is 2,47). More than 99% of these neutrons are emitted very shortly (within 10 -12 s) after the fission. These neutrons are called prompt neutrons. There are also neutrons emitted long after the fission process (sometimes several minutes later), these are called delayed neutrons. Although their ratio to the prompt neutrons is small (for the 235U they represent only 0,64% of the total fission neutrons), they are very important for controlling the nuclear chain reaction. In the first part of this measurement, we shall determine some basic parameters of the delayed neutrons. In the second part, we use the method of the delayed neutron-detection to determine the uranium content of samples (e.g. ores, soil etc.). 2. Theoretical summary There are several hundreds of ways for the 236U compound nucleus to fission. One of these possibilities is the following:

235

The number of the possible fission products is very large. Fig. 1. shows the massdistribution of the fission products. Please note that the ordinate is in logarithmic units. The curve shows two maxima: one around A = 95 and another one around A = 140. The primary fission fragments have excess neutrons as compared to the stable nuclei with the same atomic number. In most cases they undergo several successive --transitions for adjusting their neutron/proton ratio. As an example, the fragment-pair above decays as follows:

Kr 90 Rb 90 Sr 90 Y 90 Zr( stable) 33s 2,7min 28year 64h 143 Ba 143 La 143 Ce 143 Pr 143 Nd( stable) 0,5min 12min 33h 13,7d

90

The times under the arrows indicate the half-life of the corresponding - decay.

1,00E+00 1,00E-01 1,00E-02 relative yield 1,00E-03 1,00E-04 1,00E-05 1,00E-06 1,00E-07 1,00E-08 122 127 102 107 112 117 132 137 142 147 152 m ass num ber 157 72 77 82 87 92 97

1. Figure. Mass-distribution of fission products of 235U following thermal neutron induced fission 2.1. Origin of the prompt and delayed fission neutrons As it was already mentioned in the Introduction nearly all of the fission neutrons more than 99% of them are emitted just after the fission process, without considerable delay. The fission fragments that usually have much higher excitation energy than the neutron separation energy emit these prompt neutrons. The half-life of neutron-emission of these highly excited states is in the order of 1015 s or even smaller. However, not all fission fragments emit neutrons, some of them decay by emission. After the emission of the prompt neutrons usually there is no neutron emission anymore, the fission products undergo several successive -decays to reduce their neutron-excess. However, in some cases a daughter nucleus is formed after a -decay, where the excitation energy is higher than the neutron-separation energy. This nucleus will emit again a neutron, nearly promptly after its formation. These are the delayed neutrons. The decay chain is summarised as follows: A A A Z XN Z +1YN 1 Z +1TN 2 + n The X nucleus is called delayed-neutron precursor, the Y nucleus is called delayed-neutron emitter. Obviously, for these neutrons the delay time is determined by the half-life of the precursor nucleus (X), which can be quite large,

since the decay is governed by the weak interaction. Another interesting consequence of this decay chain is that the excitation energy of the delayed-neutron emitter nucleus is usually much lower than the excitation energies of the direct fission fragments. Therefore, the average energy of the delayed neutrons is also smaller (300600 keV) than that of the prompt neutrons (2 MeV in average). The total yield of the fission neutrons (average number of neutrons, is the sum of the yield of the prompt and the delayed neutrons (p, and d):

v = v p + vd

vd v .

235

Fig. 2. shows the dependence of the delayed-neutron yield for the fission-inducing neutron.

Delayed neutron yield (delayed neutrons / fission)

235

0,015 0,01

239

Pu

0,005

0,1

0,3

1,0

3,0

10,0

(MeV)

Figure 2. Delayed neutron yield in function of the energy of the fission-inducing neutron The curves show that the delayed-neutron yield is practically independent of the neutronenergy, at least in the energy interval 0 E n 4 MeV . However, the total delayed neutron yields are strongly dependent on the composition of the fissile nucleus. The values shown in Table 1 suggest two simple rules:

The delayed-neutron yield increases with the mass-number ( A), for the same atomic number (Z) The delayed-neutron yield decreases with increasing atomic number (Z). Table 1. Total delayed neutron yields (number of delayed neutrons / 100 fission events) for thermal neutron induced fission of different isotopes Fissile nucleus d (neutron/100 fissions) 233 U 0,667+0,0029 235 U 1,621+0,05 238 U* 4,39+0,10 239 Pu 0,628+0,038 240 Pu* 0,95+0,08 241 Pu 1,52+0,11 242 Pu* 2,21+0,26 *Data for fast-neutron induced fission. 2.2. The delayed neutron groups Nuclear physicists have identified so far more than 66 delayed neutron precursor nuclei.2[2] Their half-lives range between 0,12 s and 78 s, therefore their delayed neutrons appear with considerably differing delay times. A correct treatment of the delayed neutrons in reactor-kinetic calculations would consider each precursor nucleus with its own half-life and yield. However there are two problems when proceeding this way: The calculation scheme becomes complicated because of the large number of the precursor nuclei; The decay scheme, half-life and yield are not well known for every precursor nucleus. G. R. Keepin suggested an acceptable method for the calculations. In his method the experimentally determined delayed-neutrons were grouped based on the halflives of their precursors. He proceeded the same way as we are going to proceed in this measurement. He irradiated a sample made of a fissile material with neutrons. Due to the fission events a large number of precursor nuclei have been formed, which worked as a decaying delayed-neutron source after the irradiation (Sd(t)). If we denote the number of fission reactions in the sample by nf, then the number of the precursor nuclei is dnf. The Sd(t) function describes the decay of these precursor nuclei, and consequently the emission of the delayed neutrons. Fig. 3. shows such a decay curve, together with the decay curve of 87Br, which is a typical precursor nucleus.

87

Fig. 3. Time-dependence of the delayed-neutron source intensity Theoretically the Sd(t) curve is a complicated superposition of all precursors decay curve. According to Keepin, the Sd(t) function can be well approximated with a sum of 6 exponential functions:

S d (t ) = n f v di di e

i =1 6 di

t

, (2)

where di : is the yield of the i-th delayed-neutron group, di : is the decay constant of the i-th delayed-neutron group In this approximation Sd(t) represents a delayed-neutron source function, where each group has its own di delayed-neutron yield, an averaged di decay constant, and consequently, a corresponding half-life. Table 2. summarises the main parameters of the delayed-neutron groups for 3 different fissile nuclei ( 235U, 239Pu, 233U). These six delayedneutron groups are widely used in reactor kinetic calculations. Table 2. Parameters of the delayed-neutron groups for three fissile nuclei i Possible Mean Average half-life of the Delayed-neutron fraction precursor energy precursor nuclei (%) nuclei (MeV) (s) 235 239 233 235 239 233 U Pu U U Pu U 87 142 1 Br, Cs 0.25 55.72 54.28 55.0 0.021 0.0072 0.0226 137 88 2 I, Br 0.56 22.72 23.04 20.57 0.140 0.0626 0.0786 138 89 3 I, Br, 0.43 6.22 5.60 5.00 0.126 0.0444 0.0658 (93,94) Rb 139 (93,94) 4 I, Kr 0.62 2.3 2.13 2.13 0.252 0.0685 0.0730 143 (90,92) Xe, Br 140 145 5 I, Cs 0.42 0.61 0.618 0.615 0.074 0.018 0.0135 6 (Br, Rb, As 0.23 0.257 0.277 0.027 0.0093 0.0087 etc) Total 0.64 0.21 0.26

2.3. Effect of the delayed neutrons on the time-dependency of the neutron flux3[3] The discussion of the effect of delayed neutrons will involve the following assumptions: a) a) point reactor model will be chosen b) b) neutron flux and neutron density are uniform in space c) c) the neutron spectrum causing fission is a thermal one d) d) changes are propagating in the system with infinite velocity. Actually b) and d) are consequences of the choice of a point reactor model . Neutrons emitted in a fission process and maintaining the chain reaction have a certain life-cycle. They are emitted, scattered around in the reactor core, slowed down and finally they are absorbed in a fissile nucleus causing again fission. For describing the cycle we need to fix an event in the cycle as starting point. This will be the absorption of neutrons that induce fission. Let us denote the number of neutrons inducing fission in a reactor at a certain ti time by ni. In these fission events several neutrons are emitted (2,47 times more then the inducing neutrons in average). Some of them escape from the reactor, some other are absorbed by different materials (even in the fuel, but not causing fission), and only a fraction of them will cause again fission later, at ti+1 time. These latter are called the next generation of neutrons, and denoted by ni+1. The effective neutron multiplication factor is the ratio of the number of fission-inducing neutrons in succeeding n k eff = i +1 ni . If a reactor works with stationary power, then k = 1. If generations, i.e.

eff

the power increases or decreases, the effective multiplication factor differs from unity:

k eff = k eff 1

k eff k eff

k eff 1 k eff

(3)

In a stationary state = 0. The changes in the power under normal circumstances occur through nearly stationary states, therefore keff to a good approximation. n n ni n k eff = k eff 1 = i +1 1 = i +1 = ni ni n . From the definition of k we get: Therefore . Obviously n is the increase (decrease) of the total number of neutrons (n) during the life of one generation. Let us denote the

3

n = n k eff

eff

average lifetime of a neutron in the neutron-cycle by l. (Just to have an impression of the order of magnitudes, we note that in our training reactor l = 710-5 s.) As from the previous considerations follows, the time-variation of the neutron number n is given by the following differential equation: dn nk eff = dt . Supposing that keff is constant in time we get:

(4)

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