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Today were going to talk about Radioactive Processes

In this lecture, we will talk about Radioactive Equilibrium. Were going to define what we mean by Radioactive Equilibrium and identify when it occurs. Were going to look at different kinds of Radioactive Equilibrium. In particular, we will identify transient equilibrium and secular equilibrium. We will try to differentiate between them, and well give some examples of the two kinds of equilibrium. Then we will talk about activation of isotopes and look at some calculations involving activation.

Lets begin with radiation equilibrium. The phenomenon of radiation equilibrium occurs when we have a radioactive parent decaying to form a radioactive daughter. We identify different types of radiation equilibrium depending on the relationship between the half life of the daughter and the half life of the parent. If the half life of the daughter is longer than that of the parent, the activity of the daughter increases as the parent decays. When the parent is all gone, and no more daughter is produced, the amount of daughter decays with its own half life. The daughter is going to be decaying, but at a much slower rate than that of the parent. Think of it as a bath tub where the outlet allows slower water flow than the inlet lets in and say the input comes in from a tank. We fill this tub as long as we have water coming into the tub. Once we are out of input water, the water drains out of the bathtub. It turns out that this is really a trivial case. There is nothing really interesting with this form of equilibrium.

Much more interesting is the situation in which the half life of the daughter is shorter than that of the parent. The daughter is produced, but it decays rapidly. However, we will get to the point where the rate of decay of the daughter equals the rate of production of the daughter. As much daughter is being produced as is decaying. When that occurs, the activity of the daughter will appear to decay at the same rate as that of the parent. So the behavior of the daughter once this equilibrium occurs will really be the behavior of the parent as far as the radioactive decay is concerned.

Lets do a few calculations to help us understand this phenomenon. The rate of change of the number of daughter nuclei is caused by two factors, production of daughter nuclei resulting from radioactive decay of the parent, and radioactive decay of the daughter. Let dNd/dt be the rate of change of the number of daughter nuclei. This rate of change is equal to whats being produced by the parent minus whats decaying from the daughter. The rate of production of daughter from decay of the parent is the negative of the rate of decay of the parent. It is p, the transformation constant, multiplied by N0, the initial number of parent nuclei, times e to the power -p times t. What is the rate of decay of the daughter? It is equal to -d times Nd. This is our simple differential equation; all of you remember how to solve

differential equations. In fact, you are going to solve this differential equation in your problem set.

To solve the differential equation, we need a set of initial conditions. The initial conditions are that at t equals 0, the initial number of parent nuclei is equal to N0, and the initial number of daughter nuclei is zero. With these initial conditions, we solve the differential equation and we find that the number of daughter nuclei, Nd, is equal to p, the transformation constant of the parent, divided by the difference in transformation constants between that of the daughter minus that of the parent. (Remember that the shorter half life of the daughter means that the transformation constant of the daughter is greater than that of the parent, so the denominator is positive.) This quantity is multiplied by N0 times the quantity e to the -p t minus e to the -d t. So thats the solution to the differential equation that you are going to derive in the problem set.

We next make use of the fact that the activity of the parent as a function of time can be written as p times N0 times e to the - p t to obtain an expression for the number of daughter nuclei.

Finally, if we multiply both sides of the equation by d, we find that the activity of the daughter is equal to the activity of the parent times this quantity in parentheses multiplied by 1 minus e to the -(d p) t. This is how we relate the activity of the daughter to the activity of the parent. Remember, the half life of the parent is longer than the half life of the daughter, consequently the transformation constant of the daughter is greater than the transformation constant of the parent, and the quantity d p is positive.

Lets now see what happens after a long time. If t is large, we can neglect the exponential term, because it gets to be very small compared to one. So when t is large, the activity of the daughter is equal to the activity of the parent times the quantity in parentheses.

The activity of the daughter decreases with time in the with the same time dependence as the activity of the parent, that is, with an apparent half life equal to that of the parent. Notice the only time dependence in this equation is the activity of the parent, which is a function of time. So the change in activity of the daughter is really governed by the change in activity of the parent. This is then what we mean by transient equilibrium. The daughter decays at the same rate as its being produced by the parent and will decay with the half life equal to that of the parent. The quantity in parentheses, which multiplies the activity of the parent, is greater than 1, so the activity of the daughter is going to be greater than the activity of the parent.

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Given that the activity of the daughter starts out at zero and then increases, it will eventually reach a maximum value. At this point, the activity of the daughter will equal the activity of the parent. This is really the best time to extract the daughter from the parent. We can show that this optimal time is equal to the logarithm of d divided by p over d minus p.

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This graph illustrates transient equilibrium. Notice that the horizontal axis is a linear scale of time, whereas the vertical axis is a logarithmic scale of relative activity. Notice that the activity of the parent decreases in a log linear fashion. The activity of the daughter starts out at zero (minus infinity on a logarithmic scale). It increases until a point is reached where the activity of the daughter equals the activity of the parent. At this point equilibrium occurs. From this point on, we note two properties of the activity of the daughter. First of all, the activity of the daughter is greater than the activity of the parent. Secondly the activity of the daughter decreases at the same rate as the activity of the parent. Those are the two points to keep in mind when we have transient equilibrium. We will see examples of transient equilibrium in a moment.

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We have a special case of transient equilibrium, in which the half life of the parent is very much longer than the half life of the daughter. d is very much greater than p. In this case we can neglect p when it is subtracted from d. The activity of the daughter is now equal to the activity of the parent. Again, we can neglect the exponential term.

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Here is a plot of activity versus time for an example of a parent and daughter in secular equilibrium, in this case, radium decaying into radon. Radon has a half life of about three days, whereas radium has a half life of 1620 years. When equilibrium is reached, the activity of the parent and the activity of the daughter are approximately the same.

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The first applications of radon in medicine occurred when it was realized that you get the same radiation out of radon that you do with radium, but you dont have to use radium. When radium was used as a source of medical radiation, it was very expensive. The radium sources used for implants were considered to be very valuable. The idea was that you didnt want to implant the sources in the patient because there was always the possibility that you may lose the source. Not a good idea to lose the source. So if you could just capture the radon that was produced from the radium, you could then implant the radon in the patient. The appropriate radiation was given off and you still have your radium source. There was a nice article in Medical Physics some years ago that talked about the production of the first radon plant. The idea was to get the same radiation that you got from radium, but producing the radon was really cheap. The radon sources were then permanently implanted into the patient. The radon in the implanted source decays with a half life of 3.8 days. Its only in the presence of radium that it appears to decay with a half life of 1620 years. However, its neither the radium nor the radon that really produces the radiation that is used therapeutically. Several of the daughter products of radon have half lives of a fraction of a second. But, it is these daughter products in secular equilibrium with the longer-lived radon, or even radium, that produce useful gammas that we need for radiation treatment purposes.

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Again, secular equilibrium is a special case of transient equilibrium in which the half life of the daughter is very, very much less than the half life of the parent. In transient equilibrium half life of the daughter is somewhat less than the half life of the parent. The activity of the daughter is greater than the activity of the parent and decays at the same rate as the activity of the parent.

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Earlier I said that when transient equilibrium occurs, the activity of the daughter is always greater than that of the parent. I sort of lied, but not really. Here is perhaps the most common example of transient equilibrium that we use in the clinic, molybdenum 99 decaying into technetium 99m, which we use for imaging. We see here, that even though the technetium 99m is in transient equilibrium with molybdenum 99, the activity of the technetium is less than that of the parent molybdenum. The reason for this is actually quite simple. Only about 85% of the molybdenum decays via a branch that leads to the production of technetium 99m. Fifteen percent of the molybdenum decays other ways such as into the ground state of technetium 99, which we dont use for imaging purposes. So if we look at a graph of the activity of technetium 99m versus molybdenum, we see that the activity of technetium 99m is a little bit less than that of molybdenum.

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Notice also that we see that when technetium is present with molybdenum, the activity increases as we produce more and more technetium. After about two days we have reached equilibrium. Between one and two days after we begin production of technetium 99m, we remove the technetium from the generator. Because technetium has a different atomic number from that of molybdenum, it is chemically different, so we can use chemical means to separate the technetium. We remove the technetium and combine it with some kind of biologically important compound and inject it into the patient. Eventually it gets spread out in the patient and based on where it concentrates in the patient, we can find out something about whats going on inside the patient. We use technetium 99m, then, for nuclear medicine imaging. At the same time we let the technetium in the generator build up again and, typically 24 hours later, we milk the generator, pull out some more technetium and use it the next day for imaging purposes. We still use the terminology of equilibrium, and this again is an example of transient equilibrium.

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Lets talk a little bit about how we activate radioisotopes. The result really is similar to that of the production of a radioactive daughter product when the half life of the parent is much longer than that of the daughter. We will put a mass of some element into a reactor or accelerator. There is going to be a probability of an interaction of either a neutron in the reactor or a proton in the accelerator and this probability of interaction is identified by an interaction cross section.

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Conceptually, , the cross section, can be viewed as the cross section area of the nucleus as it appears to the incident particle. Its the area around the nucleus in which, if the bombarding particle enters, we will have an interaction. A large cross section means a larger area over which an interaction will occur and a higher probability of interaction.

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The rate of production of a created isotope is going to be equal to the number of atoms of the target element present times the fluence rate times the cross section. Lets talk about neutrons in particular. dN/dt, where N is the number of atoms of the created isotope, is going to be equal to the number of target atoms times the fluence rate (that is, the number of neutrons per square centimeter per second) times the cross section in centimeters squared per neutron. So, in terms of dimensional analysis we find dN/dt has the units of reciprocal seconds, number per second. And thats how we determine the rate of production of a radioactive isotope.

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Determining the number of atoms present is rather straightforward. The number of atoms present is the mass of the target times Avogadros number, which is 6.023 1023 atoms per mole, divided by the atomic weight in grams per mole. We can look up the atomic weight. We are typically given the mass in grams in that way we can determine the number of target atoms.

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Heres an example. Let us place one gram of cobalt 59 in a reactor with a neutron fluence rate of 1013 neutrons per centimeter squared per second. Lets leave the gram of cobalt 59 in the reactor for a year. How many nuclei of cobalt 60 do we get? The number of nuclei of cobalt 60 is equal to the number of nuclei of cobalt 59 times the cross section times the fluence rate times the amount of time we have left it in the reactor for activation. For now, we will ignore the decay of cobalt 60. The number of atoms of cobalt 59, we said was 1 gram times 6.023 1023 atoms per mole divided by 59 grams per mole times the cross section, which we look up in a table. We can get this number off the internet; many websites provide neutron cross sections. We find the cross section to be 37 10-24 centimeters squared. We need to multiply by the fluence rate, 1013 neutrons per square centimeter per second and multiply by the time, which is one year. We want to convert one year into seconds so we multiply by 365 times 24 times 60 times 60. We multiply everything together and we get 1.19 1020 atoms.

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We really want to determine the activity of the cobalt 60, so we multiply the number of radioactive nuclei times the transformation constant. 1.19 1020 nuclei times the transformation constant. The half life of cobalt is 5.26 years. We convert the half life into a transformation constant by dividing the half life into 0.693. 0.693 divided by 5.26 years, convert that to seconds then multiply that times 1.19 1020 and we get 4.97 1010 Becquerel. Lets convert that into Curie, for the old timers. 4.97 1010 Becquerel divided by 3.7 1010 Becquerel per Curie gives us an activity of 1.34 Curie. So we have left this one gram of cobalt 59 in a reactor for one year and the amount of cobalt 60 that we get out of the whole deal is a little more than one Curie.

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How much do we need for a cobalt teletherapy unit? A cobalt unit used radiation therapy typically used approximately 5 kCi. One thing we can do is leave the cobalt 59 source in the reactor for 5000 years but I dont think thats a good idea. An alternative is to increase the neutron fluence rate, which is really what we do. Now for some issues. Our treatment so far does not include the decay of cobalt 60, and that is a significant oversimplification. We assume a constant fluence rate thats not too bad. We neglect shielding. One atom could shield another atom and that may be important. The real issue though is the decay of cobalt 60. If we are going to leave cobalt 59 in the reactor for a year, and the half life of cobalt 60 is a little over five years, some of the cobalt 60 that forms early on is going to decay.

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So we need to add decay to the equation. dN/dt is not just equal to Nt . We also have to subtract N, which accounts for the decay of cobalt, and now we can solve the differential equation. What happens eventually is that production equals decay and we get saturation We can determine the saturation activity in a nuclear reactor by setting dN/dt equal to 0, and we find the saturation activity is Nt .

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The solution to the differential equation is that the activity of the product is equal to the saturation activity times 1 minus e to the -t. So that if we assumed no decay the e to the -t term would be zero, but we do have decay so it takes even longer. The growth of the isotope is even less. So thats some issues we need to keep in mind when we activate radioactive isotopes in a nuclear reactor.

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The final topic of this lecture is the radioactive implant. This is a situation in which we put radioactive material in place for a significant period of time. We really have two kinds of implants. We have removable implants in which we will typically use a fairly long half life material and leave the implant in place for a period of time significantly shorter than the half life. So we could pretty much neglect the radioactive decay during the implant. An example is if we implant an iridium source in a tumor. Iridium 192 has a half life of 74 days. A typical implant is left in place for a couple of days so we can approximate the activity of the iridium by assuming its constant. So thats not an issue. However, suppose we implant iodine seeds. Iodine-125 has a half life of approximately 60 days. We implant it permanently so we have to worry about how the iodine decays. How do we determine the dose delivered by a permanent implant?

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We let dD/dt be the dose rate at a point in the patient and the total dose is the integral from zero to a specified time of dD/dt. The dose rate is equal to the initial dose rate times e to the t. We look at the dose as equal to the initial dose rate times the integral from zero to t of e to the t. This is the initial dose rate divided by times 1 minus e to the t. One over turns out to be the average life or the mean life of the radioactive nucleus and it is 1.44 times the half life. So 1.44 times the half life times the initial dose rate times 1 minus e to the t is the total dose delivered by the implant.

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For an implant left in permanently t is infinity. So to determine the dose delivered by a permanent implant you take the initial dose rate and multiply it by 1.44 times the half life. Its a very simple problem. At some point you may be asked to calculate the dose delivered by an iodine 125 implant and this is how its done.

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