Nick Connor

Carbon-14 dating, known also as radiocarbon dating, is a method for determining the age of an object containing organic material by using the properties of radionuclide carbon-14. Radioactive carbon-14 has a half-life of 5730 years and undergoes β− decay, where the neutron is converted into a proton, an electron, and an electron antineutrino:

In spite of this short half-life compared to the age of the earth, carbon-14 is a naturally occurring isotope. Its presence can be explained by the following simple observation. Our atmosphere contains many gases, including nitrogen-14. Besides, the atmosphere is constantly bombarded with high energy cosmic rays, consisting of protons, heavier nuclei, or gamma rays. These cosmic rays interact with nuclei in the atmosphere, and produce also high-energy neutrons. These neutrons produced in these collisions can be absorbed by nitrogen-14 to produce an isotope of carbon-14:

Carbon-14 can also be produced in the atmosphere by other neutron reactions, including in particular 13C(n,γ)14C and 17O(n,α)14C. As a result, carbon-14 is continuously formed in the upper atmosphere by the interaction of cosmic rays with atmospheric nitrogen. On average just one out of every 1.3 x 10¹² carbon atoms in the atmosphere is a radioactive carbon-14 atom.

The resulting carbon-14 combines with atmospheric oxygen to form radioactive carbon dioxide, which is incorporated into plants by photosynthesis. Consequently, all biological systems as  plants, animals and humans contain a certain level of radioactive carbon-14. As long as the biological system is alive the level is constant due to constant intake of all isotopes of carbon. When the biological system dies, it stops exchanging carbon with its environment, and from that point onwards the amount of carbon-14 it contains begins to decrease as the carbon-14 undergoes radioactive decay. On the other hand, the amount of stable carbon-12 remains unchanged. As a result, the relative concentration of these two isotopes in any organism changes after its death. The method enables datings to be made up to about 20,000 years ago with an accuracy of about ±100 years.

The technique of carbon dating was suggested initially by Willard Libby and his colleagues in 1949. In 1960, Willard Libby was awarded the Nobel Prize in chemistry for this work.

See also:

Radiometric Dating

Radiometric dating (or radioactive dating) is any technique used to date organic and also inorganic materials from a process involving radioactive decay. The method compares the abundance of a naturally occurring radioactive isotope within the material to the abundance of its decay products, which form at a known constant rate of decay.

All these methods are based on the fact the rate at which radioactive nuclei disintegrate is unaffected by their environment, it can be used to estimate the age of any material sample or object which contains a radioactive isotope. Calculations of the decay of radioactive nuclei are relatively straightforward, owing to the fact that there is only one fundamental law governing all decay process.

The radioactive decay law states that the probability per unit time that a nucleus will decay is a constant, independent of time. This constant is called the decay constant and is denoted by λ, “lambda”. This constant probability may vary greatly between different types of nuclei, leading to the many different observed decay rates. The radioactive decay of certain number of atoms (mass) is exponential in time.

Radioactive decay law: N = N₀.e^-λt

Among the best-known techniques are:

• carbon-14 dating,
• potassium–argon dating,
• uranium–lead dating.

Radiometric dating methods are used in geochronology to establish the geologic time scale and can be also used to date archaeological materials, including ancient artifacts.

Carbon-14 Dating – Radiocarbon Dating

Carbon-14 dating, known also as radiocarbon dating, is a method for determining the age of an object containing organic material by using the properties of radionuclide carbon-14. Radioactive carbon-14 has a half-life of 5730 years and undergoes β− decay, where the neutron is converted into a proton, an electron, and an electron antineutrino:

In spite of this short half-life compared to the age of the earth, carbon-14 is a naturally occurring isotope. Its presence can be explained by the following simple observation. Our atmosphere contains many gases, including nitrogen-14. Besides, the atmosphere is constantly bombarded with high energy cosmic rays, consisting of protons, heavier nuclei, or gamma rays. These cosmic rays interact with nuclei in the atmosphere, and produce also high-energy neutrons. These neutrons produced in these collisions can be absorbed by nitrogen-14 to produce an isotope of carbon-14:

Carbon-14 can also be produced in the atmosphere by other neutron reactions, including in particular 13C(n,γ)14C and 17O(n,α)14C. As a result, carbon-14 is continuously formed in the upper atmosphere by the interaction of cosmic rays with atmospheric nitrogen. On average just one out of every 1.3 x 10¹² carbon atoms in the atmosphere is a radioactive carbon-14 atom.

The resulting carbon-14 combines with atmospheric oxygen to form radioactive carbon dioxide, which is incorporated into plants by photosynthesis. Consequently, all biological systems as  plants, animals and humans contain a certain level of radioactive carbon-14. As long as the biological system is alive the level is constant due to constant intake of all isotopes of carbon. When the biological system dies, it stops exchanging carbon with its environment, and from that point onwards the amount of carbon-14 it contains begins to decrease as the carbon-14 undergoes radioactive decay. On the other hand, the amount of stable carbon-12 remains unchanged. As a result, the relative concentration of these two isotopes in any organism changes after its death. The method enables datings to be made up to about 20,000 years ago with an accuracy of about ±100 years.

The technique of carbon dating was suggested initially by Willard Libby and his colleagues in 1949. In 1960, Willard Libby was awarded the Nobel Prize in chemistry for this work.

Age of the Earth – Uranium-lead Dating

The age of the Earth is about 4.54 billion years. This dating is based on evidence from radiometric age-dating of meteorite material and is consistent with the radiometric ages of the oldest-known terrestrial and lunar samples.

One of the oldest radiometric dating methods is uranium-lead dating. The age of the earth’s crust can be estimated from the ratio between the amounts of uranium-238 and lead-206 found in geological specimens. The long half-life of the isotope uranium-238 (4.51×10⁹ years) makes it well-suited for use in estimating the age of the earliest igneous rocks and for other types of radiometric dating, including uranium–thorium dating and uranium–uranium dating.

Uranium-lead dating is based on the measurement of the first and the last member of the uranium series, which is one of three classical radioactive series beginning with naturally occurring uranium-238. This radioactive decay chain consists of unstable heavy atomic nuclei that decay through a sequence of alpha and beta decays until a stable nucleus is achieved. In case of uranium series, the stable nucleus is lead-206. The assumption made is that all the lead-206 nuclei found in the specimen today were originally uranium-238 nuclei.  That means at the crust’s formation the specimen contained no lead-206 nuclei. If no other lead isotopes are found in the specimen, this is a reasonable assumption. Under this condition, the age of the sample can be calculated by assuming exponential decay of uranium-238. That is:

Uranium-lead dating method is usually performed on the mineral zircon. Zircons from Jack Hills in Western Australia, have yielded U-Pb ages up to 4.404 billion years, interpreted to be the age of crystallization, making them the oldest minerals so far dated on Earth.

See also:

Radioactive Decay

Decay Law – Equation – Formula

The radioactive decay law states that the probability per unit time that a nucleus will decay is a constant, independent of time. This constant is called the decay constant and is denoted by λ, “lambda”. This constant probability may vary greatly between different types of nuclei, leading to the many different observed decay rates. The radioactive decay of certain number of atoms (mass) is exponential in time.

Radioactive decay law: N = N.e^-λt

The rate of nuclear decay is also measured in terms of half-lives. The half-life is the amount of time it takes for a given isotope to lose half of its radioactivity. If a radioisotope has a half-life of 14 days, half of its atoms will have decayed within 14 days. In 14 more days, half of that remaining half will decay, and so on. Half lives range from millionths of a second for highly radioactive fission products to billions of years for long-lived materials (such as naturally occurring uranium). Notice that short half lives go with large decay constants. Radioactive material with a short half life is much more radioactive (at the time of production) but will obviously lose its radioactivity rapidly. No matter how long or short the half life is, after seven half lives have passed, there is less than 1 percent of the initial activity remaining.

The radioactive decay law can be derived also for activity calculations or mass of radioactive material calculations:

(Number of nuclei) N = N.e^-λt     (Activity) A = A.e^-λt      (Mass) m = m.e^-λt

, where N (number of particles) is the total number of particles in the sample, A (total activity) is the number of decays per unit time of a radioactive sample, m is the mass of remaining radioactive material.

Decay Constant and Half-Life – Equation – Formula

In calculations of radioactivity one of two parameters (decay constant or half-life), which characterize the rate of decay, must be known. There is a relation between the half-life (t_1/2) and the decay constant λ. The relationship can be derived from decay law by setting N = ½ N_o. This gives:

where ln 2 (the natural log of 2) equals 0.693. If the decay constant (λ) is given, it is easy to calculate the half-life, and vice-versa.

Bateman Equations

In physics, the Bateman equations are a set of first-order differential equations, which describe the time evolution of nuclide concentrations undergoing serial or linear decay chain. The model was formulated by Ernest Rutherford in 1905 and the analytical solution for the case of radioactive decay in a linear chain was provided by Harry Bateman in 1910. This model can be also used in nuclear depletion codes to solve nuclear transmutation and decay problems.

For example, ORIGEN is a computer code system for calculating the buildup, decay, and processing of radioactive materials. ORIGEN uses a matrix exponential method to solve a large system of coupled, linear, first-order ordinary differential equations (similar to the Bateman equations) with constant coefficients.

The Bateman equations for radioactive decay case of n – nuclide series in linear chain describing nuclide concentrations are as follows:

Example – Radioactive Decay Law

A sample of material contains 1 mikrogram of iodine-131. Note that, iodine-131 plays a major role as a radioactive isotope present in nuclear fission products, and it a major contributor to the health hazards when released into the atmosphere during an accident. Iodine-131 has a half-life of 8.02 days.

Calculate:

1. The number of iodine-131 atoms initially present.
2. The activity of the iodine-131 in curies.
3. The number of iodine-131 atoms that will remain in 50 days.
4. The time it will take for the activity to reach 0.1 mCi.

Solution:

1. The number of atoms of iodine-131 can be determined using isotopic mass as below.

N_I-131 = m_I-131 . N_A / M_I-131

N_I-131 = (1 μg) x (6.02×10²³ nuclei/mol) / (130.91 g/mol)

N_I-131 = 4.6 x 10¹⁵ nuclei

2. The activity of the iodine-131 in curies can be determined using its decay constant:

The iodine-131 has half-live of 8.02 days (692928 sec) and therefore its decay constant is:

Using this value for the decay constant we can determine the activity of the sample:

3) and 4) The number of iodine-131 atoms that will remain in 50 days (N_50d) and the time it will take for the activity to reach 0.1 mCi can be calculated using the decay law:

As can be seen, after 50 days the number of iodine-131 atoms and thus the activity will be about 75 times lower. After 82 days the activity will be approximately 1200 times lower. Therefore, the time of ten half-lives (factor 2¹⁰ = 1024) is widely used to define residual activity.

See also:

Radioactive Equilibrium

In physics, the Bateman equations are a set of first-order differential equations, which describe the time evolution of nuclide concentrations undergoing serial or linear decay chain. The model was formulated by Ernest Rutherford in 1905 and the analytical solution for the case of radioactive decay in a linear chain was provided by Harry Bateman in 1910. This model can be also used in nuclear depletion codes to solve nuclear transmutation and decay problems.

For example, ORIGEN is a computer code system for calculating the buildup, decay, and processing of radioactive materials. ORIGEN uses a matrix exponential method to solve a large system of coupled, linear, first-order ordinary differential equations (similar to the Bateman equations) with constant coefficients.

The Bateman equations for radioactive decay case of n – nuclide series in linear chain describing nuclide concentrations are as follows:

Bateman Equations for Nuclear Transmutation

As was written, this model can be also used in nuclear depletion codes to solve nuclear transmutation and decay problems as well. In case of transmutation the decay constants that govern Bateman equations for a decay case are substituted by transmutation constants. By the transmutation constant λ_i,j we understand probability of the ith nuclide production per time unit from the jth nuclide destruction, as a result of nuclear interaction with the whole spectrum of interacting particles or due to the natural nuclear decay.

These equations are usually used for the exact evolution of isotopic changes in the nuclear fuel during fuel depletion. Fuel depletion is usually modelled mathematically as a set of differential equations known as evolution equations.

Special Reference: Jerzy Cetnar, General solution of Bateman equations for nuclear transmutations. Annals of Nuclear Energy 33 (2006). January 2006.

See also:

Radioactive Equilibrium

In physics of nuclear decays, a radioactive equilibrium exists when a radioactive nuclide is decaying at the same rate at which it is being produced. The disintegrating nucleus is usually referred to as the parent nucleus and the nucleus remaining after the event as the daughter nucleus. The daughter nucleus can either be stable or radioactive. If it is radioactive, then it decays into a daughter nucleus and so on. Thus, each radioactive parent nucleus can initiate a series of decays, with each decay-product having its own characteristic decay constant.

Concentration of daughter nuclei in the radioactive equilibrium depends primarily on proportions of half-lives (or decay constants) of parent and daughter nuclei. Since the production rate and decay rate are equal, the number of atoms present remains constant over time. In any case, a radioactive equilibrium is not established immediately, but it only takes place after a transition period. This period is of the order of few half-lifes of the longest-lived nucleus in the decay chain. In case of radioactive decay chains, a radioactive equilibrium may be established between each member of the decay chain.

As was written, proportionality of half-lives is a key parameter, which determines type of radioactive equilibrium:

• Radioactive equilibrium is not established when a half-life of the parent nucleus is shorter than a half-life of the daughter nucleus. In this case the production rate and decay rate of certain member of decay chain cannot be equal.
• Secular radioactive equilibrium exists when the parent nucleus has an extremely long half-life. This type of equilibrium is particularly important in nature. Over the 4.5 billion years of the Earth’s history, especially uranium 238, uranium 235 and thorium 232 and members of their decay chains have reached radioactive equilibria between the parent nucleus and the various descendants.
• Transient radioactive equilibrium exists when a half-life of the parent nucleus is longer than a half-life of the daughter nucleus. In this case, the parent nuclide and the daughter nuclide decay at essentially the same rate.

Transient Radioactive Equilibrium

The transient radioactive equilibrium exists when a half-life of the parent nucleus is longer than a half-life of the daughter nucleus, but the concentration of parent nuclei significantly decreases in time. In this case, the parent nuclide and the daughter nuclide may decay at essentially the same rate, but both concentrations of nuclides decreases as the concentration of parent nuclei decreases. Contrary to secular equilibrium, the half-life of the daughter nuclei is not negligible compared to parent’s half-life.

An example of this type of compound decay process is a Technetium-99m generator producing technetium-99m for nuclear medicine diagnostic procedures from molybdenum-99. Technetium-99m’s short half-life of 6 hours makes storage impossible and would make transport very expensive. Therefere, for medical purposes, molybdenum-99 is used to produce technetium-99m. These two isotopes are in the transient equilibrium. The decay constant for molybdenum-99 is considerably smaller than the decay constant for technetium-99m. Although the decay constant for molybdenum-99 is smaller, the actual rate of decay is initially larger than that of molybdenum-99 because of the great difference in their initial concentrations. As the concentration of the daughter increases, the rate of decay of the daughter will approach and eventually match the decay rate of the parent. When this occurs, they are said to be in the transient equilibrium. In case of  Technetium-99m generator, transient equilibrium occurs after about four half-lives. Today, technetium-99m is the most utilized element in nuclear medicine and is employed in a wide variety of nuclear medicine imaging studies.

Also the transient equilibrium can occasionally be disrupted when one of the intermediary nuclei leaves the sample where its ancestors are confined.

Transient Radioactive Equilibrium with Source – Example

A special example of radioactive equilibrium are concentrations of iodine-135 and xenon-135 in a nuclear reactor, but in this case, the xenon burnup must be taken into account. Note that, in this special case, the half-life of the parent nucleus is shorter than the half-life of the daughter nucleus. The production and removal of xenon can be characterized by the following differential equations:

When the rate of production of iodine equals the rate of removal of iodine, equilibrium exists. This equilibrium also known as “xenon 135 reservoir”, since all of this iodine must undergo a decay to xenon. In equilibrium, the iodine concentration remains constant and is designated N_I(eq). The following equation for the iodine equilibrium concentration can be determined from the preceding equation by setting the dN_I/dt =0. Since the equilibrium iodine concentration is proportional to the fission reaction rate, it is also proportional to reactor power level.

When the rate of production of xenon 135 equals the rate of removal, equilibrium exists also for xenon. The xenon concentration remains constant and is designated N_Xe(eq). The following equation (1) for the xenon equilibrium concentration can be determined from the preceding equation by setting the dN_Xe/dt =0. For xenon 135 to be in equilibrium, iodine 135 must also be in equilibrium. Substituting the expression for equilibrium iodine 135 concentration into the equation for equilibrium xenon (1) results in the following (2).

From this equation it can be seen that the equilibrium value for xenon 135 increases as power increases, because the numerator is proportional to the fission reaction rate. But the thermal flux is also in the denominator. Therefore, as the thermal flux exceeds some value, the xenon burnup begins to dominate, and at approximately 10¹⁵ neutrons.cm^-2.s^-1, the xenon-135 concentration approaches a limiting value. The equilibrium iodine 135 and xenon 135 concentrations as a function of neutron flux are illustrated in the following figure.

See also:

Radioactive Equilibrium

In physics of nuclear decays, a radioactive equilibrium exists when a radioactive nuclide is decaying at the same rate at which it is being produced. The disintegrating nucleus is usually referred to as the parent nucleus and the nucleus remaining after the event as the daughter nucleus. The daughter nucleus can either be stable or radioactive. If it is radioactive, then it decays into a daughter nucleus and so on. Thus, each radioactive parent nucleus can initiate a series of decays, with each decay-product having its own characteristic decay constant.

Concentration of daughter nuclei in the radioactive equilibrium depends primarily on proportions of half-lives (or decay constants) of parent and daughter nuclei. Since the production rate and decay rate are equal, the number of atoms present remains constant over time. In any case, a radioactive equilibrium is not established immediately, but it only takes place after a transition period. This period is of the order of few half-lifes of the longest-lived nucleus in the decay chain. In case of radioactive decay chains, a radioactive equilibrium may be established between each member of the decay chain.

As was written, proportionality of half-lives is a key parameter, which determines type of radioactive equilibrium:

• Radioactive equilibrium is not established when a half-life of the parent nucleus is shorter than a half-life of the daughter nucleus. In this case the production rate and decay rate of certain member of decay chain cannot be equal.
• Secular radioactive equilibrium exists when the parent nucleus has an extremely long half-life. This type of equilibrium is particularly important in nature. Over the 4.5 billion years of the Earth’s history, especially uranium 238, uranium 235 and thorium 232 and members of their decay chains have reached radioactive equilibria between the parent nucleus and the various descendants.
• Transient radioactive equilibrium exists when a half-life of the parent nucleus is longer than a half-life of the daughter nucleus. In this case, the parent nuclide and the daughter nuclide decay at essentially the same rate.

Secular Equilibrium

Secular radioactive equilibrium exists when the parent nucleus has an extremely long half-life. Secular equilibrium is typical for natural radioactive series, such as the thorium series or the uranium series. For the uranium series with uranium-238 (with a half-life of 4.47 billion years), where all of the elements in the chain are in secular equilibrium, each of the descendants has built up to an equilibrium amount and all decay at the rate set by the original parent. The only exception is the final stable element (lead-206) on the end of the chain. Its number of atoms is constantly increasing. In any case, a radioactive equilibrium is not established immediately, but it only takes place after a transition period. This period is of the order of few half-lifes of the longest-lived nucleus in the decay chain (²³⁴U for the uranium series; ²³¹Pa for the actinium series). In case of radioactive decay chains, a radioactive equilibrium may be established between each member of the decay chain.

As can be seen,  the secular equilibrium is particularly important in nature. Over the 4.5 billion years of the Earth’s history, especially uranium 238, uranium 235 and thorium 232 and members of their decay chains have reached radioactive equilibria between the parent nucleus and the various descendants. The half-lives of all their descendants are all extremely variable, and it is difficult to represent a range of timescales going from individual seconds to millions of years. Since daughter radioisotopes have different half-lives then secular equilibrium is reached after some time. In the long decay chain for a naturally radioactive element, such as uranium-238, where all of the elements in the chain are in secular equilibrium, each of the descendants has built up to an equilibrium amount and all decay at the rate set by the original parent. If and when equilibrium is achieved, each successive daughter isotope is present in direct proportion to its half-life (or to its decay constant).

Since its activity is inversely proportional to its half-life, each nuclide in the decay chain finally contributes as many individual transformations as the head of the chain. Radioactive cascade in the secular equilibrium significantly influences radioactivity (disintegrations per second) of natural samples and natural materials. All the descendants are present, at least transiently, in any natural sample, whether metal, compound, or mineral. For example, pure uranium-238 is weakly radioactive (proportional to its long half-life), but a uranium ore is about 13 times more radioactive (approximately 13 descendants in the decay chain) than the pure uranium-238 metal because of its daughter isotopes (e.g. radon, radium etc.) it contains. Not only are unstable radium isotopes significant radioactivity emitters, but as the next stage in the decay chain they also generate radon, a heavy, inert, naturally occurring radioactive gas. Moreover the decay heat of uranium and its decay products (e.g. radon, radium etc.) contributes to heating of Earth’s core. Together with thorium and potassium-40 in the Earth’s mantle is thought that these elements are the main source of heat that keeps the Earth’s core liquid.

The secular equilibrium can occasionally be disrupted when one of the intermediary nuclei leaves the sample (e.g. radon released from soil) where its ancestors are confined. These local disruptions are important to consider in the use of dating techniques. Disruption of the secular equilibrium also influences radioactivity of fresh nuclear fuel. Most of PWRs use the uranium fuel, which is in the form of uranium dioxide. But this uranium dioxide must be chemically purified and most of its decay chain is not present in the fresh nuclear fuel.

Radioactive Equilibrium of Uranium-234

Isotope of uranium-234 is a member of the uranium series. This isotope has the half-life of only 2.46×10⁵ years and therefore it do not belong to primordial nuclides (unlike ²³⁵U and ²³⁸U). On the other hand, this isotope is still present in the Earth’s crust, but this is due to the fact ²³⁴U is an indirect decay product of ²³⁸U. ²³⁸U decays via alpha decay into ²³⁴U. ²³⁴U decays via alpha decay into 230Th, except very small fraction (on the order of ppm) of nuclei which decays by spontaneous fission.

In a natural sample of uranium, these nuclei are present in the unalterable proportions of the radioactive equilibrium of the ²³⁸U filiation at a ratio of one atom of ²³⁴U for about 18 500 nuclei of ²³⁸U. As a result of this equilibrium these two isotopes (²³⁸U and ²³⁴U) contribute equally to the radioactivity of natural uranium.

See also:

Radioactive Equilibrium

In physics of nuclear decays, a radioactive equilibrium exists when a radioactive nuclide is decaying at the same rate at which it is being produced. The disintegrating nucleus is usually referred to as the parent nucleus and the nucleus remaining after the event as the daughter nucleus. The daughter nucleus can either be stable or radioactive. If it is radioactive, then it decays into a daughter nucleus and so on. Thus, each radioactive parent nucleus can initiate a series of decays, with each decay-product having its own characteristic decay constant.

Concentration of daughter nuclei in the radioactive equilibrium depends primarily on proportions of half-lives (or decay constants) of parent and daughter nuclei. Since the production rate and decay rate are equal, the number of atoms present remains constant over time. In any case, a radioactive equilibrium is not established immediately, but it only takes place after a transition period. This period is of the order of few half-lifes of the longest-lived nucleus in the decay chain. In case of radioactive decay chains, a radioactive equilibrium may be established between each member of the decay chain.

As was written, proportionality of half-lives is a key parameter, which determines type of radioactive equilibrium:

• Radioactive equilibrium is not established when a half-life of the parent nucleus is shorter than a half-life of the daughter nucleus. In this case the production rate and decay rate of certain member of decay chain cannot be equal.
• Secular radioactive equilibrium exists when the parent nucleus has an extremely long half-life. This type of equilibrium is particularly important in nature. Over the 4.5 billion years of the Earth’s history, especially uranium 238, uranium 235 and thorium 232 and members of their decay chains have reached radioactive equilibria between the parent nucleus and the various descendants.
• Transient radioactive equilibrium exists when a half-life of the parent nucleus is longer than a half-life of the daughter nucleus. In this case, the parent nuclide and the daughter nuclide decay at essentially the same rate.

Secular Equilibrium

Secular radioactive equilibrium exists when the parent nucleus has an extremely long half-life. Secular equilibrium is typical for natural radioactive series, such as the thorium series or the uranium series. For the uranium series with uranium-238 (with a half-life of 4.47 billion years), where all of the elements in the chain are in secular equilibrium, each of the descendants has built up to an equilibrium amount and all decay at the rate set by the original parent. The only exception is the final stable element (lead-206) on the end of the chain. Its number of atoms is constantly increasing. In any case, a radioactive equilibrium is not established immediately, but it only takes place after a transition period. This period is of the order of few half-lifes of the longest-lived nucleus in the decay chain (²³⁴U for the uranium series; ²³¹Pa for the actinium series). In case of radioactive decay chains, a radioactive equilibrium may be established between each member of the decay chain.

As can be seen,  the secular equilibrium is particularly important in nature. Over the 4.5 billion years of the Earth’s history, especially uranium 238, uranium 235 and thorium 232 and members of their decay chains have reached radioactive equilibria between the parent nucleus and the various descendants. The half-lives of all their descendants are all extremely variable, and it is difficult to represent a range of timescales going from individual seconds to millions of years. Since daughter radioisotopes have different half-lives then secular equilibrium is reached after some time. In the long decay chain for a naturally radioactive element, such as uranium-238, where all of the elements in the chain are in secular equilibrium, each of the descendants has built up to an equilibrium amount and all decay at the rate set by the original parent. If and when equilibrium is achieved, each successive daughter isotope is present in direct proportion to its half-life (or to its decay constant).

Since its activity is inversely proportional to its half-life, each nuclide in the decay chain finally contributes as many individual transformations as the head of the chain. Radioactive cascade in the secular equilibrium significantly influences radioactivity (disintegrations per second) of natural samples and natural materials. All the descendants are present, at least transiently, in any natural sample, whether metal, compound, or mineral. For example, pure uranium-238 is weakly radioactive (proportional to its long half-life), but a uranium ore is about 13 times more radioactive (approximately 13 descendants in the decay chain) than the pure uranium-238 metal because of its daughter isotopes (e.g. radon, radium etc.) it contains. Not only are unstable radium isotopes significant radioactivity emitters, but as the next stage in the decay chain they also generate radon, a heavy, inert, naturally occurring radioactive gas. Moreover the decay heat of uranium and its decay products (e.g. radon, radium etc.) contributes to heating of Earth’s core. Together with thorium and potassium-40 in the Earth’s mantle is thought that these elements are the main source of heat that keeps the Earth’s core liquid.

The secular equilibrium can occasionally be disrupted when one of the intermediary nuclei leaves the sample (e.g. radon released from soil) where its ancestors are confined. These local disruptions are important to consider in the use of dating techniques. Disruption of the secular equilibrium also influences radioactivity of fresh nuclear fuel. Most of PWRs use the uranium fuel, which is in the form of uranium dioxide. But this uranium dioxide must be chemically purified and most of its decay chain is not present in the fresh nuclear fuel.

Radioactive Equilibrium of Uranium-234

Isotope of uranium-234 is a member of the uranium series. This isotope has the half-life of only 2.46×10⁵ years and therefore it do not belong to primordial nuclides (unlike ²³⁵U and ²³⁸U). On the other hand, this isotope is still present in the Earth’s crust, but this is due to the fact ²³⁴U is an indirect decay product of ²³⁸U. ²³⁸U decays via alpha decay into ²³⁴U. ²³⁴U decays via alpha decay into 230Th, except very small fraction (on the order of ppm) of nuclei which decays by spontaneous fission.

In a natural sample of uranium, these nuclei are present in the unalterable proportions of the radioactive equilibrium of the ²³⁸U filiation at a ratio of one atom of ²³⁴U for about 18 500 nuclei of ²³⁸U. As a result of this equilibrium these two isotopes (²³⁸U and ²³⁴U) contribute equally to the radioactivity of natural uranium.

Transient Radioactive Equilibrium

The transient radioactive equilibrium exists when a half-life of the parent nucleus is longer than a half-life of the daughter nucleus, but the concentration of parent nuclei significantly decreases in time. In this case, the parent nuclide and the daughter nuclide may decay at essentially the same rate, but both concentrations of nuclides decreases as the concentration of parent nuclei decreases. Contrary to secular equilibrium, the half-life of the daughter nuclei is not negligible compared to parent’s half-life.

An example of this type of compound decay process is a Technetium-99m generator producing technetium-99m for nuclear medicine diagnostic procedures from molybdenum-99. Technetium-99m’s short half-life of 6 hours makes storage impossible and would make transport very expensive. Therefere, for medical purposes, molybdenum-99 is used to produce technetium-99m. These two isotopes are in the transient equilibrium. The decay constant for molybdenum-99 is considerably smaller than the decay constant for technetium-99m. Although the decay constant for molybdenum-99 is smaller, the actual rate of decay is initially larger than that of molybdenum-99 because of the great difference in their initial concentrations. As the concentration of the daughter increases, the rate of decay of the daughter will approach and eventually match the decay rate of the parent. When this occurs, they are said to be in the transient equilibrium. In case of  Technetium-99m generator, transient equilibrium occurs after about four half-lives. Today, technetium-99m is the most utilized element in nuclear medicine and is employed in a wide variety of nuclear medicine imaging studies.

Also the transient equilibrium can occasionally be disrupted when one of the intermediary nuclei leaves the sample where its ancestors are confined.

Transient Radioactive Equilibrium with Source – Example

A special example of radioactive equilibrium are concentrations of iodine-135 and xenon-135 in a nuclear reactor, but in this case, the xenon burnup must be taken into account. Note that, in this special case, the half-life of the parent nucleus is shorter than the half-life of the daughter nucleus. The production and removal of xenon can be characterized by the following differential equations:

When the rate of production of iodine equals the rate of removal of iodine, equilibrium exists. This equilibrium also known as “xenon 135 reservoir”, since all of this iodine must undergo a decay to xenon. In equilibrium, the iodine concentration remains constant and is designated N_I(eq). The following equation for the iodine equilibrium concentration can be determined from the preceding equation by setting the dN_I/dt =0. Since the equilibrium iodine concentration is proportional to the fission reaction rate, it is also proportional to reactor power level.

When the rate of production of xenon 135 equals the rate of removal, equilibrium exists also for xenon. The xenon concentration remains constant and is designated N_Xe(eq). The following equation (1) for the xenon equilibrium concentration can be determined from the preceding equation by setting the dN_Xe/dt =0. For xenon 135 to be in equilibrium, iodine 135 must also be in equilibrium. Substituting the expression for equilibrium iodine 135 concentration into the equation for equilibrium xenon (1) results in the following (2).

From this equation it can be seen that the equilibrium value for xenon 135 increases as power increases, because the numerator is proportional to the fission reaction rate. But the thermal flux is also in the denominator. Therefore, as the thermal flux exceeds some value, the xenon burnup begins to dominate, and at approximately 10¹⁵ neutrons.cm^-2.s^-1, the xenon-135 concentration approaches a limiting value. The equilibrium iodine 135 and xenon 135 concentrations as a function of neutron flux are illustrated in the following figure.

Bateman Equations

In physics, the Bateman equations are a set of first-order differential equations, which describe the time evolution of nuclide concentrations undergoing serial or linear decay chain. The model was formulated by Ernest Rutherford in 1905 and the analytical solution for the case of radioactive decay in a linear chain was provided by Harry Bateman in 1910. This model can be also used in nuclear depletion codes to solve nuclear transmutation and decay problems.

For example, ORIGEN is a computer code system for calculating the buildup, decay, and processing of radioactive materials. ORIGEN uses a matrix exponential method to solve a large system of coupled, linear, first-order ordinary differential equations (similar to the Bateman equations) with constant coefficients.

The Bateman equations for radioactive decay case of n – nuclide series in linear chain describing nuclide concentrations are as follows:

Bateman Equations for Nuclear Transmutation

As was written, this model can be also used in nuclear depletion codes to solve nuclear transmutation and decay problems as well. In case of transmutation the decay constants that govern Bateman equations for a decay case are substituted by transmutation constants. By the transmutation constant λ_i,j we understand probability of the ith nuclide production per time unit from the jth nuclide destruction, as a result of nuclear interaction with the whole spectrum of interacting particles or due to the natural nuclear decay.

These equations are usually used for the exact evolution of isotopic changes in the nuclear fuel during fuel depletion. Fuel depletion is usually modelled mathematically as a set of differential equations known as evolution equations.

Special Reference: Jerzy Cetnar, General solution of Bateman equations for nuclear transmutations. Annals of Nuclear Energy 33 (2006). January 2006.

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Radioactive Decay

The neptunium series is a radioactive series beginning with neptunium-237. Its members are produced artificially by nuclear reactions and do not occur naturally, because the half-life of the longest lived isotope in the series is short compared to the age of the earth. This radioactive decay chain consists of unstable heavy atomic nuclei that decay through a sequence of alpha and beta decays until a stable nucleus is achieved. In case of neptunium series, the stable nucleus is bismuth-209 (with half-life of 1.9E19 years) and thallium-205.

Since alpha decay represents the disintegration of a parent nucleus to a daughter through the emission of the nucleus of a helium atom (which contains four nucleons), there are only four decay series. Within each series, therefore, the mass number of the members may be expressed as four times an appropriate integer (n) plus the constant for that series. As a result, the neptunium series is known as the 4n+1 series.

The total energy released from neptunium-237 to thallium-205, including the energy lost to neutrinos, is 50.0 MeV.

In some kind of smoke detectors, you can meet radionuclides from this series. Ionization smoke detectors usually use a radioisotope, typically americium-241, to ionize air and to detect smoke. In this case americium-241 decays to neptunium-237 and is, in fact, a member of neptunium series.

Types of Decay in Neptunium Series

Within each radioactive series, there are two main modes of radioactive decay:

• Alpha decay. Alpha decay represents the disintegration of a parent nucleus to a daughter through the emission of the nucleus of a helium atom. Alpha particles consist of two protons and two neutrons bound together into a particle identical to a helium nucleus. Because of its very large mass (more than 7000 times the mass of the beta particle) and its charge, it heavy ionizes material and has a very short range.
• Beta decay. Beta decay or β decay represents the disintegration of a parent nucleus to a daughter through the emission of the beta particle. Beta particles are high-energy, high-speed electrons or positrons emitted by certain types of radioactive nuclei such as potassium-40. The beta particles have greater range of penetration than alpha particles, but still much less than gamma rays.The beta particles emitted are a form of ionizing radiation also known as beta rays. The production of beta particles is termed beta decay.

See also:

Radioactive Series

The actinium series, known also as the actinium cascade, is one of three classical radioactive series beginning with naturally occurring uranium-235. This radioactive decay chain consists of unstable heavy atomic nuclei that decay through a sequence of alpha and beta decays until a stable nucleus is achieved. In case of actinium series, the stable nucleus is lead-207.

Since alpha decay represents the disintegration of a parent nucleus to a daughter through the emission of the nucleus of a helium atom (which contains four nucleons), there are only four decay series. Within each series, therefore, the mass number of the members may be expressed as four times an appropriate integer (n) plus the constant for that series. As a result, the actinium series is known as the 4n+3 series.

The total energy released from uranium-235 to lead-207, including the energy lost to neutrinos, is 46.4 MeV.

Activity of Natural Samples – Actinium Series

Actinium cascade influences radioactivity (disintegrations per second) of natural samples and natural materials, although, in this case activity of natural samples is determined primarily by uranium-238. Uranium-235, which alone constitutes 0.72% of natural uranium has half-life of 7.04×10⁸ years (6.5 times shorter than the isotope 238) and therefore its abundance is lower than ²³⁸U(99.28%). All the descendants of uranium-235 and uranium-238 are present, at least transiently, in any natural uranium-containing sample, whether metal, compound, or mineral. For example, pure uranium-238 is weakly radioactive (proportional to its long half-life), but a uranium ore is about 13 times more radioactive than the pure uranium-238 metal because of its daughter isotopes (e.g. radon, radium etc.) it contains. Not only are unstable radium isotopes significant radioactivity emitters, but as the next stage in the decay chain they also generate radon, a heavy, inert, naturally occurring radioactive gas. Moreover the decay heat of uranium and its decay products (e.g. radon, radium etc.) contributes to heating of Earth’s core. Together with thorium and potassium-40 in the Earth’s mantle is thought that these elements are the main source of heat that keeps the Earth’s core liquid.

Types of Decay in Actinium Series

Within each radioactive series, there are two main modes of radioactive decay:

• Alpha decay. Alpha decay represents the disintegration of a parent nucleus to a daughter through the emission of the nucleus of a helium atom. Alpha particles consist of two protons and two neutrons bound together into a particle identical to a helium nucleus. Because of its very large mass (more than 7000 times the mass of the beta particle) and its charge, it heavy ionizes material and has a very short range.
• Beta decay. Beta decay or β decay represents the disintegration of a parent nucleus to a daughter through the emission of the beta particle. Beta particles are high-energy, high-speed electrons or positrons emitted by certain types of radioactive nuclei such as potassium-40. The beta particles have greater range of penetration than alpha particles, but still much less than gamma rays.The beta particles emitted are a form of ionizing radiation also known as beta rays. The production of beta particles is termed beta decay.

See also:

Radioactive Series

The uranium series, known also as radium series, is one of three classical radioactive series beginning with naturally occurring uranium-238. This radioactive decay chain consists of unstable heavy atomic nuclei that decay through a sequence of alpha and beta decays until a stable nucleus is achieved. In case of uranium series, the stable nucleus is lead-206.

Since alpha decay represents the disintegration of a parent nucleus to a daughter through the emission of the nucleus of a helium atom (which contains four nucleons), there are only four decay series. Within each series, therefore, the mass number of the members may be expressed as four times an appropriate integer (n) plus the constant for that series. As a result, the uranium series is known as the 4n+2 series.

The total energy released from uranium-238 to lead-206, including the energy lost to neutrinos, is 51.7 MeV.

Uranium Series and Uranium-234

Isotope of uranium-234 is a member of this series. This isotope has the half-life of only 2.46×10⁵ years and therefore it do not belong to primordial nuclides (unlike ²³⁵U and ²³⁸U). On the other hand, this isotope is still present in the Earth’s crust, but this is due to the fact ²³⁴U is an indirect decay product of ²³⁸U. ²³⁸U decays via alpha decay into ²³⁴U. ²³⁴U decays via alpha decay into 230Th, except very small fraction (on the order of ppm) of nuclei which decays by spontaneous fission.

In a natural sample of uranium, these nuclei are present in the unalterable proportions of the radioactive equilibrium of the ²³⁸U filiation at a ratio of one atom of ²³⁴U for about 18 500 nuclei of ²³⁸U. As a result of this equilibrium these two isotopes (²³⁸U and ²³⁴U) contribute equally to the radioactivity of natural uranium.

Activity of Natural Samples – Uranium Series

Uranium cascade significantly influences radioactivity (disintegrations per second) of natural samples and natural materials. All the descendants are present, at least transiently, in any natural uranium-containing sample, whether metal, compound, or mineral. For example, pure uranium-238 is weakly radioactive (proportional to its long half-life), but a uranium ore is about 13 times more radioactive than the pure uranium-238 metal because of its daughter isotopes (e.g. radon, radium etc.) it contains. Not only are unstable radium isotopes significant radioactivity emitters, but as the next stage in the decay chain they also generate radon, a heavy, inert, naturally occurring radioactive gas. Moreover the decay heat of uranium and its decay products (e.g. radon, radium etc.) contributes to heating of Earth’s core. Together with thorium and potassium-40 in the Earth’s mantle is thought that these elements are the main source of heat that keeps the Earth’s core liquid.

Types of Decay in Uranium Series

Within each radioactive series, there are two main modes of radioactive decay:

• Alpha decay. Alpha decay represents the disintegration of a parent nucleus to a daughter through the emission of the nucleus of a helium atom. Alpha particles consist of two protons and two neutrons bound together into a particle identical to a helium nucleus. Because of its very large mass (more than 7000 times the mass of the beta particle) and its charge, it heavy ionizes material and has a very short range.
• Beta decay. Beta decay or β decay represents the disintegration of a parent nucleus to a daughter through the emission of the beta particle. Beta particles are high-energy, high-speed electrons or positrons emitted by certain types of radioactive nuclei such as potassium-40. The beta particles have greater range of penetration than alpha particles, but still much less than gamma rays.The beta particles emitted are a form of ionizing radiation also known as beta rays. The production of beta particles is termed beta decay.

See also:

Radioactive Series