Comments Secular

on Equilibrium, Equilibrium

Transient

Equilibrium, Decay

and

in Serial
John R. Prince

Radioactive

King Faisal Specialist

Hospital

and Research

Centre,

Rivadh,

Saudi Arabia

Equations describing serial radioactive decay are reviewed along with published descriptions of transient and secular equilibrium. It is shown that terms describing equilibrium are not used in the same way by various authors. Specijk definitions are proposed; they suggest that secular equilibrium is a subset of transient equilibrium.

J Nuci Med 20: 162-164, 1979

Equilibrium is used to describe the condition where the deny ative of a function is equal to zero. In radioactive decay it relates to the situation where the number of atoms of a particular kind does not change with time. Clearly, this is a contradiction, since radioactive decay implies change, whereas equilibrium does not. Whereas absolute equilibrium is not possible, equilibrium is ad equately approximated in many important situations whenever the parent species is substantially longer-lived than the daughter nuclides. The various approximations to equilibrium give rise to terms transient equilibrium and secular equilibrium . These terms, however, are not used in a consistent way in physics textbooks (I -4) and they appear to have been applied improperly in some reference works (510). a result of this discordant informa As tion, considerable confusion exists in some technical personnel who do not deal with these concepts regularly, especially when these concepts are applied to available generator systems. As an example, it is not uncommon for examination review ques tions to be phrased something like the following. A radionu clide generator system is described by the term I) tran sient equilibrium, 2) secular equilibrium, etc.(1112). this As
communication will show, the response to such a question will

XI

the

radioactive

decay

constant

for

atoms

of

the

first

species; etc. When there are only three nuclear species, which is of pnmary
importance to nuclear medicine, the differential equations de

scribing the decay and buildup of the various nucides are (1) dN1 dN,

_@i_= -A1N1,

(1)
(2)

-@ii= A1N1 A2N2,and

dt A2N2.

dN3

(3)

When only Species 1 is present initially, the standard solutions

are:

N1 = N2 = N3=N15(l @1 N1'(e@ e@), and +A

Al

(4) (5)
(6)

@ @,

depend upon the reference books consulted and, hence, upon the individual's training. From this brief review it is hoped that
whatever confusion exists will be dispelled and a more consistent

_@1e

A2

A2 A1

usage of terms and concepts may emerge. Consider serial radioactive decay where Species I decays only to Species 2, which in turn decays only to Species 3, and so on until finally a stable product is formed. The following definitions will be used:
0 = the number of atoms of the first species at time zero;

Consider three special cases in the discussion of Eq. 5, which

relates to the buildup generator system. and decay of the first daughter in the

Relatively shoi@t-IIved arentA1 > A@ Since A p -

@2-in the ,

N1 = the number of atoms of the first species atany time

Received Oct. 20, 1977; revision accepted Oct. 3, 1978

John R. Prince, Dept. of Medical Physics, King Faisal Spe cialist Hospital and Research Centre, P.O. Box 3354, Riyadh,

Saudi Arabia.

present case A1> A2, and the amount of daughter element, N2, will increase with time until it goes through a maximum. Even tually, when the parent element has decayed away, the daughter element will decay with its own characteristic half-life. There are no commercially available radionucide generators that possess the characteristic of A@ A2. However, Brucer (13) > has observed that such generator systems may be useful, point in8 out an example, which he termed a reverse cow, in the commercial production of 1-131. Quoting from Brucer, In the early days of the large-scale production of 1-131, reactor pro THE JOURNAL OF NUCLEAR MEDICINE

162

TECHNICAL NOTE

duction time was purchased for tellurium irradiation in a Cana wedian approximate the useful life of the generator. However, if reactor. During shipment to American pharmaceuticalrestrict withhouses, our attention to time spans that are long compared the In-ll3m8-day 1.3-day tellurium parent decayed to the desiredthe half-life of the daughter element, then the Sn-1l3 e 1-131 daughter, which was readily separated. Bruceris a good example where e@ an be approximated by I. Equa c further comments these reverse cowsmay be useful in pro asducing tion 5 can then be written for any generator a label that originates at the site of deposition of another label. A similar suggestion was made by Spencer and Hosain in e@). (12) N2 = A2decay a discussion of generator systems with approximately equalFA1N1(1 isestablished constants for parent and daughter (14). No equilibrium 0,been longer times, when e@t e under these conditions and no descriptive term hasAt it.Relatively suggestedto denote FA1N1 long-lived parentT1> T2 (A@< A2). For suffi (13) N, ciently large values of t, e@t will be negligibly small compared A,with
e@. Under these circumstances, Eq. 5 is approximated

byAt becomes(7)If N2 2A1 A

@

still longer times, when e@'t ....@ but we can no longer 0 approximate e@ y I, Eq. 13 b FA1N1@@1i
A,

at sufficiently large values oft, Eq. 7 predicts that N, will appearN, CombiningorEqs.4and7weget: half-life ofthe parent. decay with the characteristic
A5for

A,to the parent and daughter elements remain undisturbed then

(14)

condition where Eq. 13 is a valid approximation to Eq. 1,2,3),Equationof t.The 5 is generally referred to as secular equilibrium (e.g., large values Eq.pendent 8 predicts that eventually a constant ratio, mdc although not by all authors (e.g., 3,17). Most authors stop at alThis of time, will be established between N, and N1.13 in their derivation of secular equilibrium, but Acosta et 15.with condition, where N,/N1 is constant but both decrease(4) have carried their derivation on to Eq. (1)and time, is referred to as transient equilibrium by Kaplan andDISCUSSIONAndrews Hendee (2) but is called secular equilibrium by Lapp common to define secular equilibrium as that condition where the activities of the parent and the daughter are equal. Further, most authors either implicitly or explicitly define sec ular equilibrium as that condition when the parent and are equal and there is no important decay of the parent A2 A2 (9)activities during the period of interest implied in the definition. Notice A1 A2 A1 thatEquation that Eq. 11, which refers to transient equilibrium, shows 9 predicts that, given Special Case B and a longwith atime, a judicious choice of F, one could theoretically describe 1, the activity of Species 2 will always be greater than that pair where parent and daughter activities remain of Species I. equal even though substantial decay of the parent may take An example of the application of Eqs. 5, 6, and 9 is given by plane during the period of interest. This definition would then the Te-l32 e 1-132 generator (2). Interestingly, most of the include secular equilibrium as a subset of transient equilibrium. reference books consulted (510),but not all (3), have apparently No example of this theoretical possibility comes to mind. applied these equations to the Mo-99 . Tc-99m generator, since If one defines transient equilibrium as that condition where a most of the books do show that the activity of Tc-99m exceeds constant ratio of activities obtains but the parent decays appre that of Mo-99 at large times. ciably during the period of interest, then one must also define In order to make Eq. 5 general for any generator system, such what is meant by the term, period f interest. Clearly, for o as the Mo-99 Tc-99m generator, the fraction, F, of Species long time spans, all parent nucides in generator systems decay 1 decaying directly to Species 2 must be taken into account. appreciably. However, if one defines the period of interest as Thenparent-daughter parentN, several elution periods, then most generator systems have that do not decay appreciably. For example, everyone A1N1@@'t F approach: they do not define a transient equilibrium but do define a secular equilibrium (see Eqs. 1316). Since the activity A = AN, it follows from Eq. 8 thatis daughter. everyoneandmay scnbed by the term transient quilibrium; but not e the(11)Sn-ll3 agree on the appropriate term used for describing .- In-113m generator. FA2 Based upon the information in this communication, the fol A1 A, A1@ definitions are proposed, in the belief that they are com Package inserts from the manufacturers of generators and sev patible with the nmjority of applications. eral literature sources (e.g., 2,14,15) are available, and provide Transient equilibrium is that condition in serial radioactive the correct technical information for the Mo-99 -. Tc-99m gen daughterExtremely decay where the ratio of activities of the parent and erator.lowing
(3). Acosta et al. (4) seem to take an intermediate

N2 N1

A1 A2 1 A

(15) (8)@=F

A, A1nucides

(10)

may agree

that the Mo-99 .Tc-99m

generator

could

be de

is constant. The mathematical definition is given long-lived parentT1 T,. Here A1 4 A,, and 711.e condition we can approximate A, 1 by A, andradionucides by Eqs. under this A y@ 1. For by radioactivenot radionucide geherators this latter assumption isSecular equilibrium is that condition in serial true for long time spans (A, t # 0), i.e., time spans thatdecay where the ratio of activities of the parent and daughter

Volume 20, Number 2

163

PRINCE

radionucides is a constant and where there is no important decay of the parent nucide during the time interval of interest. Secular equilibrium should be considered as a subset of tran sient equilibrium. The mathematical definition is given by Eqs. 12 and 13. (Note that in such a secular equilibrium the activity of the daughter nuclide is also essentially constant.) In accordance with the above definitions, all radionucide gen erators in current use in nuclear medicine can achieve transient equilibrium. Most of them, but not all, can be described by both the terms transient equilibrium and secular equilibrium if the time of interest is restricted to a few elution periods rather than the life of the generator or historical time. REFERENCES I . KAPLAN I: Nuclear Physics, 2nd ed. Cambridge, Mass, Addison-Wesley Publishing Co., Inc., 1964, pp 244248 Book Medical Publishers, Inc. , 1973, pp 46-49
3. LAPP RE, ANDREW HL Nuclear Radiation Physics, 4th

6. EARLYPJ, RAZZAKMA, SODEE DB: Textbook of Nuclear Medicine Technology, 2nd ed. Saint Louis, C.V. Mosby Co., 1975, p 77
7. LANGE RC: Nuclear Medicine for Technicians, Chicago,

Yearbook Medical Publishers, Inc., 1973, p 50 8. JOHNSHE, CUNNINGHAM Jfl The Physics of Radiology, 3rd ed. Springfield, Ill, Charles C. Thomas, 1969,p 92 9. QUIMBY EH, FEITELBERG GROSS RadioactiveNu 5, W:
clides in Medicine and Biology: Basic Physics and Instrumen tation, 3rd ed. Philadelphia, Lea and Febiger, 1970, p 72 10. CHANDRA R: Introductory Physics of Nuclear Medicine.

Philadelphia, Lea and Febiger, 1976, p 45

11. SOLOMON NA Nuclear Medicine. Medical Examination

Review Book, vol. 25. Flushing, N.Y., Medical Examination Publishing Company, Inc., p 24
12. Farv GD, KLOBUKOWSKI CJ: Nuclear Medicine Tech nology Examination Review Book. Flushing, N.Y., Medical Ex amination Publishing Company, Inc., 1974, p 56 13. BRUCER M: 118 Medical radioisotope cows. Isotopes Ra diat Technol 3: 112, 965 1

.2. WR Physics. HENDEEChicago, MedicalYear Radiation

Isotopes 27: 5758,1976 New York, of Nuclear Harper and Row, Medicine. 1973, pp 389391 W.P. Saunders

/4. SPENCER RP, HOSAINF: Radionucide generatorswith equal decay constants for parent and daughter. mt J AppI Rad

ed Englewood Cliffs, NJ: Prentice-Hall, 1972, pp 187189 4. ACOSTA COWANCL, GRAHAM Essentialsof Mod V., BJ:
em Physics. Principles

15. ALLEN JF: An improved technetium generator for mcd ical applications. mt i Applied Rad Isotopes 16: 332334, 965 1
16. LAMSON M, HOTrE CE, ICE RD: Practical Generator Ki

5. WAGNERHN, RHODES Bk The Radiopharmaceutical. In

Philadelphia,

netics. J Nucl Med Technol 4: 2127, 976 1

17. ANDREWS HL Radiation Biophysics, 2nd ed. Englewood

Co., 1968, p 267

Cliffs, N.J. , Prentice-Hall, Inc., 1974, p 172

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