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Radioactive Decay Kinetics RDCH 702

Radioactive Decay Kinetics RDCH 702. Outline Radioactive decay kinetics Basic decay equations Utilization of equations Mixtures Equilibrium Branching Natural radiation Dating. Introduction. Number of radioactive nuclei that decay in a sample decreases with time Exponential decrease

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Radioactive Decay Kinetics RDCH 702

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  1. Radioactive Decay KineticsRDCH 702 Outline • Radioactive decay kinetics • Basic decay equations • Utilization of equations • Mixtures • Equilibrium • Branching • Natural radiation • Dating

  2. Introduction • Number of radioactive nuclei that decay in a sample decreases with time • Exponential decrease • Independent of P, T, mass action • Conditions associated with chemical kinetics • Electron capture and internal conversion can be affected by conditions • Specific for isotope • Irreversible • Decay of given radionuclide is random • Statistical • Evaluate behavior of group

  3. Basic Decay Equations • Decay is 1st order • Rate proportional to amount of parent isotope • Equal to the rate of isotope disintegration • Proportional to number of radioactive nuclei • rate of decay=decay constant*# radioactive nuclei • A=lN • Decay constant is average decay probability per nucleus for a unit time • Represented by l

  4. probability of disintegration independent past history and present circumstances depends only on length of time interval Probability of decay: p=Dt Probability of not decaying: 1-p=1- Dt (1- Dt)n=probability that atom will survive n intervals of Dt nDt=t, therefore (1-  Dt)n =(1-  t/n)n limn∞(1+x/n)n=ex, (1- t/n)n=e-t is limiting value Considering No initial atoms fraction remaining unchanged after time t is N/No= e-t N is number of atoms remaining at time t Basic decay equations N=Noe-t

  5. Radioactivity as Statistical Phenomenon: Error from Counting • Binomial Distribution for Radioactive Disintegrations • Probability W(m) of obtaining m disintegrations in time t from No original radioactive atoms • For radioactive disintegration • p=1-e-t • Average number M of atoms disintegrating in time t is M=No(1-e-t) • For small t, M=Not and disintegration R=M/t=No • Small t means count time is short compared to half life • Corresponds to -dN/dt=N • Expected Standard Deviation • M is number of counts • Relative error = s-1 • What is a reasonable number of counts for an experiment? • More counts, lower error

  6. Measured Activity • In practicality, activity (A) is used instead of the number of atoms (N). • A= ct, m • where c is the detection coefficient • A=AOe-t • Units • Curie • 3.7E10 decay/s • 1 g Ra • Becquerel • 1 decay/s

  7. Half Life and decay constant Half-life is time needed to decrease nuclides by 50% Relationship between t1/2 and l N/No=1/2=e-t ln(1/2)=-t1/2 ln 2= t1/2 t1/2=(ln 2)/

  8. Half lives • Large variation in half-lives for different isotopes • Short half-lives can be measured • Evaluate activity over time • Observation on order of half-life • Long half-lives • Based on decay rate and sample • Need to know total amount of nuclide in sample • A=ln • A is activity, n is number of nuclei

  9. Exponential Decay • Average Life () for a radionuclide • found from sum of times of existence of all atoms divided by initial number of nuclei • 1/l=1/(ln2/t1/2)=1.443t1/2=t • Average life greater than half life by factor of 1/0.693 • during time 1/ activity reduced to 1/e it’s initial value

  10. Lifetime • Total number of nuclei that decay over time • Dose • Atom at a time • Couple with Heisenberg uncertainty principle • DE Dt≥h/2p • Dt is t • with energy in eV • DE≥(4.133E-15 eV s/2p)/ t= G • G is decay width • Resonance energy • t1/2=1 sec, t=1.44 s, G=4.56E-16 eV

  11. Width and energy • Need very short half-lives for large widths • Useful in Moessbauer spectroscopy • Absorption distribution is centered around Eg+DE • emission centered Eg-DE . • overlapping part of the peaks can be changed by changing the temperature of the source and/or the absorber.

  12. Equations • Nt=Noe-lt • N=number of nuclei, l= decay constant, t=time • Also works for A (activity) or C (counts) • At=Aoe-lt, Ct=Coe-lt • A= lN • 1/l=1/(ln2/t1/2)=1.443t1/2=t

  13. Half-life calculation Using Nt=Noe-lt • For an isotope the initial count rate was 890 Bq. After 180 minutes the count rate was found to be 750 Bq • What is the half-life of the isotope • 750=890exp(-l*180 min) • 750/890=exp(-l*180 min) • ln(750/890)= -l*180 min • -0.171/180 min= -l • 9.5E-4 min-1=l=ln2/t1/2 • t1/2=ln2/9.5E-4=729.6 min

  14. Half-life calculation A=lN • A 0.150 g sample of 248Cm has a alpha activity of 0.636 mCi. • What is the half-life of 248Cm? • Find A • 0.636 E-3 Ci (3.7E10 Bq/Ci)=2.35E7 Bq • Find N • .150 g x 1 mole/248 g x 6.02E23/mole= 3.64E20 atoms • l=A/N= 2.35E7 Bq/3.64E20 atoms=6.46E-14 s-1 • t1/2=ln2/l=0.693/6.46E-14 s-1=1.07E13 s • 1.07E13 s=1.79E11 min=2.99E9 h=1.24E8 d =3.4E5 a

  15. Counting A=lN • Your gamma detector efficiency at 59 keV is 15.5 %. What is the expected gamma counts from 75 micromole of 241Am? • Gamma branch is 35.9 % for 241Am • C=(0.155)(0.359)lN • t1/2=432.7 a* (3.16E7 s/a)=1.37E10 s • l=ln2/1.37E10 s=5.08E-11 s-1 • N=75E-6 moles *6.02E23/mole=4.52E19 atoms • C=(0.155)(0.359)5.08E-11 s-1*4.52E19 =1.28E8 Bq

  16. Decay Scheme

  17. Specific activity • Activity of a given amount of radionuclide • Use A=lN • Use of carrier should be included • SA of 226Ra • 1 g 226Ra, t1/2= 1599 a • 1 g * 1 mole/226 g * 6.02E23 atoms/mole = 2.66E21 atom = N • t1/2=1599 a *3.16E7 s/a = 5.05E10 s • l=ln2/ 5.05E10 s =1.37E-11 s-1 • A= 1.37E-11 s-1 * 2.66E21=3.7E10 Bq

  18. Specific Activity • 1 g 244Cm, t1/2=18.1 a • 1 g * 1 mole/244 g * 6.02E23 atoms/mole = 2.47E21 atom = N • t1/2=18.1 a *3.16E7 s/a = 5.72E8 s • l=ln2/ 5.72E8 s =1.21E-9 s-1 • A= 1.21E-9 s-1 * 2.47E21=2.99E12 Bq • Generalized equation for 1 g • 6.02E23/Isotope mass *2.19E-8/ t1/2 (a) • 1.32E16/(Isotope mass* t1/2 (a))

  19. Specific Activity

  20. Specific Activity • Activity/mole • N=6.02E23 • SA (Bq/mole) of 129I, t1/2=1.57E7 a • t1/2=1.57E7 a *3.16E7 s/a = 4.96E14 s • l=ln2/ 4.96E14 s =1.397E-15 s-1 • A= 1.397E-15 s-1 *6.02E23=8.41E8 Bq • Generalized equation • SA (Bq/mole)=1.32E16/t1/2 (a)

  21. Specific Activity

  22. SA with carrier • 1E6 Bq of 152Eu is added to 1 mmole Eu. • Specific activity of Eu (Bq/g) • Need to find g Eu • 1E-3 mole *151.96 g/mole = 1.52E-1 g • =1E6 Bq/1.52E-1 g =6.58E6 Bq/g • =1E9 Bq/mole • What is SA after 5 years • t1/2=13.54 a • = 6.58E6*exp((-ln2/13.54)*5)= • 5.09E6 Bq/g

  23. Lifetime • Atom at a time chemistry • 261Rf lifetime • Find the lifetime for an atom of 261Rf • t1/2 = 65 s • t=1.443t1/2 • t=93 s • Determines time for experiment • Method for determining half-life

  24. Mixtures of radionuclides • Composite decay • Sum of all decay particles • Not distinguished by energy • Mixtures of Independently Decaying Activities • if two radioactive species mixed together, observed total activity is sum of two separate activities: A=A1+A2=c11N1+c22N2 • any complex decay curve may be analyzed into its components • Graphic analysis of data is possible

  25. l=0.554 t1/2=1.25 hr l=0.067 t1/2=10.4 hr Can determine initial concentration and half-life of each radionuclide

  26. Parent – daughter decay • Isotope can decay into radioactive isotope • Uranium decay series • Lower energy • Different properties • A • Z • Spin • Parity • For a decay parent -> daughter • Rate of daughter formation dependent upon parent decay rate- daughter decay rate

  27. Parent - daughter • For the system 1 decays into 2 • Rearranging gives • Solve and substitute for N1 using N1t=N1oe-lt • Linear 1st order differential equation • Solve by integrating factors • Multiply by el2t

  28. Parent-daughter • Integrate from t 0->t • Multiply by e-l2tand solve for N2 Decay of initial daughter Growth of daughter from parent

  29. Parent daughter relationship • Can solve equation for activity from A=lN • Find maximum daughter activity based on dN/dt=0 • Solve for t • For 99mTc (t1/2=6.01 h) from 99Mo (2.75 d), find time for maximum daughter activity • lTc=2.8 d-1, lMo=0.25 d-1

  30. Half life relationships • Can simplify relative activities based on half life relationships • No daughter decay • No activity of daughter • Number of daughter atoms due to parent decay • No Equilibrium • if parent is shorter-lived than daughter (12), no equilibrium attained at any time • daughter reaches maximum activity when 1N1=2N2 • All parents decay, then decay is based on daughter

  31. Half life relationships • Transient equilibrium • Parent half life greater than 10 x daughter half life • (1 < 2) • Parent daughter ratio becomes constant over time • As t goes toward infinity

  32. Half life relationship • Secular equilibrium • Parent much longer half-life than daughter • 1E4 times greater (1 << 2) • Parent activity does not measurably decrease in many daughter half-lives

  33. Many Decays • Bateman solution • Only parent present at time 0

  34. Branching decay • Branching Decay • partial decay constants must be considered • A has only one half life • if decay chain branches and two branches are later rejoined, the two branches are treated as separate chains • production of common member beyond branch point is sum of numbers of atoms formed by the two paths • Branching ratio is based on relative constants • li/lt

  35. Branching Decay • For a branching decay of alpha and beta • At=Aa+Ab • A=lN, so • ltN=laN+lbN; lt=la+lb • 1=Aa /At+Ab /At; 1=la /lt+lb /lt • Consider 212Bi, what is the half life for each decay mode? • Alpha branch 36 %, beta branch 64 % • t1/2=60.55 min • lt=0.0114; 0.36=la /lt; 0.36=la /0.0114; la=0.0041 • t1/2alpha = 169 min • lt=la+lb; 0.0114=0.0041+lb; 0.0073=lb • t1/2beta = 95.0 min

  36. Natural Radionuclides • 70 naturally occurring radioactive isotopes • Mainly decay from actinides • Tritium • 14C • 40K • 70 kg “reference man,” • 4400 Bq of 40K • 3600 Bq of 14C • US diet • 1 pCi/day of 238U, 226Ra, and 210Po • air • ~ 0.15 pCi/L of 222Rn • earth’s crust • ~10 ppm and ~4 ppm of the radioelements Th and U. • interior heat budget of the planet Earth is dominated by the contributions from the radioactive decay of U, Th, and K

  37. Production of radionuclides • R=N0sf • s=cross section • f=neutron flux • To full consider produced nuclei need saturation factor • Account for decay during production • (1-e-(lt)) • t=time of irradiation, decay constant of product • If the disintegration rate of radioactive product at end bombardment is divided by saturation factor, the formation rate obtained • R=A/(1-e-(lt))

  38. Environmental radionuclides • primordial nuclides that have survived since the time the elements were formed • t1/2>1E9 a • Decay products of these long lived nuclides • 40K., 87Rn, 238U, 235U, 232Th • cosmogenic are shorter lived nuclides formed continuously by the interaction of comic rays with matter • 3H., 14C, 7Be • 14N(n, 1H)14C (slow n) • 14N(n, 3H)12C (fast n) • anthropogenic are nuclides introduced into the environment by the activities of man • Actinides and fission products • 14C and 3H

  39. Dating • Radioactive decay as clock • Based on Nt=Noe-lt • Solve for t • N0 and Nt are the number of radionuclides present at times t=0 and t=t • Nt from A = λN • t the age of the object • Need to determine No • For decay of parent P to daughter D total number of nuclei is constant

  40. Dating • Pt=Poe-lt • Measuring ratio of daughter to parent atoms • no daughter atoms present at t=0 • that they are all due to the parent decay • none have been lost during time t • A mineral has a 206Pb/238U =0.4. What is the age of the mineral? • t=(1/(ln2/4.5E9))ln(1+0.4) • 2.2E9 years

  41. Dating • 14C dating • Based on constant formation of 14C • No longer uptakes C upon organism death • 227 Bq 14C/kgC at equilibrium • What is the age of a wooden sample with 0.15 Bq/g C? • t=(1/(ln2/5730 a))*ln(0.227/0.15)=3420 a

  42. Dating • Determine when Oklo reactor operated • Today 0.7 % 235U • Reactor 3.5 % 235U • Compare 235U/238U (Ur) ratios and use Nt=Noe-lt

  43. Questions • Make excel sheets to calculate • Activity to mass • Calculate specific activity • Should also consider • Concentration and volume to activity • Determine activity for counting • Parent to progeny • Daughter and granddaughter • i.e., 239U to 239Np to 239Pu

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