on the interpretation of errors in counting experiments
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On The Interpretation Of Errors In CountingExperimentsLloyd A. Currie a ba Physikalisches Institut der Universität Bern , 3000, Bern, Switzerlandb Analytical Chemistry , Division National Bureau of Standards , Washington, D. C., 20234Published online: 05 Dec 2006.
To cite this article: Lloyd A. Currie (1971) On The Interpretation Of Errors In Counting Experiments, Analytical Letters, 4:12,873-882, DOI: 10.1080/00032717108066074
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ANALYTICAL LETTERS, 4(12), 873-882 (1971)
ON THE INTERPRETATION O F ERRORS I N
COUNTING EXPERIMENTS
KEY WORDS: r a d i o a c t i v i t y , a c t i v a t i o n a n a l y s i s , Binomial and Poisson d i s t r i b u t i o n s , compound d i s t r i b u t i o n s , chi-squared, d i s p e r s i o n t e s t .
Lloyd A. C u r r i e
Phys ika l i s ches I n s t i t u t d e r U n i v e r s i t a t Bern 3000 Bern, Switzer land
and
A n a l y t i c a l Chemistry Divis ion Na t iona l Bureau of Standards Washington, D. C. 20234
ABSTRACT
D i g i t a l experiments, such as t h e measurement of r ad io -
a c t i v i t y , are u s u a l l y c h a r a c t e r i z e d by random e r r o r s which
fol low t h e Binomial o r Poisson d i s t r i b u t i o n . Three types of
d i f f i c u l t y which commonly a r i s e i n t h e s t a t i s t i c a l t r ea tmen t
of such experiments i nc lude :
a ) f a i l u r e t o recognize t h a t t h e u n c e r t a i n t y i n t h e p h y s i c a l
q u a n t i t y of i n t e r e s t may be governed by a compound proba-
b i l i t y d i s t r i b u t i o n , p a r t i c u l a r l y when d e a l i n g with s h o r t -
l i v e d r a d i o a c t i v i t y ;
b ) t h e improper use of t h e chi-squared s t a t i s t i c when making
s t anda rd error estimates i n weighted l eas t - squa res calcu-
l a t i o n s ;
c) s e l e c t i n g t h e c o r r e c t number of degrees of freedom and
choosing between t h e x2 d i s p e r s i o n t e s t and t h e goodness-
o f - f i t t e s t f o r grouped d a t a .
873
Copyright @ 1971 by Marcel Dekker, Inc. NO PART of this work may be reproduced or utilized in any form or by any means, electronic or mechanical, including xerography, photocopying, microfilm, and re- cording, or by any information storage and retrieval system, without the written permission of the publisher.
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L. A. CURRIE
Examination of t h e n a t u r e of each of t h e s e d i f f i c u l t i e s has
been followed by a recommended cour se of a c t i o n .
INTRODUCTION
P h y s i c a l measurements which a r e fundamentally d i g i t a l i n
n a t u r e - i . e . , "count ing" experiments - may f r e q u e n t l y
be i n t e r p r e t e d i n terms of t h e Poisson d i s t r i b u t i o n . The
most common such measurement p rocesses are t h o s e invo lv ing
r a d i o a c t i v i t y or n u c l e a r r e a c t i o n s . However, s e v e r a l o t h e r
t ypes of a n a l y t i c a l measurement which invo lve p u l s e coun t ing ,
such as m a s s spectrometry and e l e c t r o n microprobe a n a l y s i s ,
a l s o f a l l i n t o t h i s class.
Assessment of t h e p r e c i s i o n and ( s t a t i s t i c a l ) f i t of t h e
r e s u l t s of such experiments g e n e r a l l y p r e s e n t s no d i f f i c u l t y .
Three s p e c i a l problems, however, f r e q u e n t l y g e n e r a t e confusion
and erroneous conc lus ions . In t h e f i r s t of t h e s e , s t a n d a r d
e r r o r s are o f t e n underest imated because on ly t h e l a s t (Binomial)
s t a g e of a m u l t i s t a g e (Compound) p rocess i s cons ide red , and t h e
Index of Dispersion (variance/mean) i s consequent ly f a l s e l y
assumed t o be less than u n i t y . The second problem relates
t o t h e improper use of x2 t o " c o r r e c t " t h e s t a n d a r d e r r o r
estimate i n weighted l eas t - squa res c a l c u l a t i o n s . A simple
m u l t i p l i c a t i v e c o r r e c t i o n i s s e e n t o apply on ly when t h e
r e l a t i v e weights ( i n v e r s e v a r i a n c e s ) a r e known i n advance.
F i n a l l y , one may be f aced wi th t h e problem of dec id ing
between t h e goodness-of-f i t test based upon t h e observed
d i s p e r s i o n and t h e ( d i s t r i b u t i o n - f r e e ) t e s t based upon t h e
observed (vs expected) f r e q u e n c i e s f o r grouped d a t a , and - i n e i t h e r case - d e c i d i n g upon t h e c o r r e c t number of degrees
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INTERPRETATION OF ERRORS IN COUNTING EXPERIMENTS
of freedom. In what fol lows w e s h a l l a t tempt t o expose t h e
sou rces of d i f f i c u l t y and t o s u g g e s t t h e proper t r ea tmen t
f o r each of t h e s e problems.
COMPOUND DISTRIBUTIONS
Random e r r o r s a r i s i n g i n t h e measurement of r a d i o a c t i v i t y
are g e n e r a l l y considered t o fol low t h e Binomial d i s t r i b u t i o n .
This conclusion fol lows provided t h a t one has a l a r g e number
( N ) of e q u i v a l e n t r a d i o a c t i v e n u c l e i having an e q u a l proba-
b i l i t y (p ) t o decay and be d e t e c t e d . For a simple d e r i v a t i o n ,
one may c o n s u l t a s t anda rd t e x t such as t h e one by F r i ed lande r , where t h e l i m i t i n g Poisson ( p < < l ) and Normal ( p c < l , Np>>l)
d i s t r i b u t i o n s are a l s o deduced.
1
A b a s i c d i s t i n c t i o n between t h e Binomial case and i t s
Poisson l i m i t relates t o t h e va r i ance . Although, i n e i t h e r
case t h e mean i s Np, t h e va r i ance e q u a l s Np(1-p) f o r t h e
Binomial d i s t r i b u t i o n , b u t Np ( t h e mean) f o r t h e Poisson
d i s t r i b u t i o n . Therefore , experiments i n which r ad ionuc l ides
are observed with high e f f i c i e n c y f o r a p e r i o d t h a t i s n o t
s h o r t compared t o t h e mean l i f e may l e a d t o s i g n i f i c a n t
dec reases i n t h e va r i ance from t h e Poisson va lue , due t o t h e
f a c t o r , (1-p) . This conclusion -- t h a t t h e va r i ance is
smaller than t h e mean -- has been noted by many au tho r s i n
connection with experiments i nvo lv ing s h o r t - l i v e d radio-
a c t i v i t y l r 2 .
t h e s t anda rd d e v i a t i o n of t h e r e s u l t of an experiment i n
a c t i v a t i o n a n a l y s i s i s d e r i v e d from t h e expres s ion f o r t h e
v a r i a n c e of t h e Binomial d i s t r i b u t i o n , Np(1-p) I with N and
p d e f i n e d as above.
In r e f e r e n c e 2 (Eq ' s . 2 4 and 2 5 ) , f o r example,
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L. A . CURRIE
Herein lies an error. Although t h e v a r i a n c e , Np(1-p) ,
prope r ly r e l a t e s t o t h e i n i t i a l number of r a d i o a c t i v e n u c l e i
i n a given, a c t i v a t e d sample, it does n o t re la te t o t h e b a s i c
q u a n t i t y of i n t e r e s t -- t h e o r i g i n a l number of s t a b l e n u c l e i
(No) . r e l e v a n t s t a t i s t i c a l t h e o r y has been developed by Feller . Following F e l l e r ' s development, w e may c o n s i d e r t h e o v e r a l l
act ivat ion-decay-count ing p rocess as a compound p rocess , i n
which t h e f i r s t s t e p ( a c t i v a t i o n ) is a Poisson process and
succeeding s t e p s a r e simply b i n a r y ( B e r n o u l l i ) t r i a l s (decay/no
decay, count/no coun t , e t c . ) Feller t r ea t s t h e problem by
d e r i v i n g t h e d i s t r i b u t i o n of t h e sum,
3 This d i s t i n c t i o n has been noted by Stevenson4 and t h e 5
s = x 1 + x 2 + x 3 + + %
where N as w e l l as each of t h e x ' s are independent, random
v a r i a b l e s . The mean (us) and va r i ance (Vs) of S are given by,
- ' s - 'N'x
2 - vs - PNVx + VNIJX
Taking t h e case of n u c l e a r a c t i v a t i o n , where S r e p r e s e n t s
t h e number of counts ob ta ined and x = 0,l f o r each of t h e N
r a d i o a c t i v e atoms -- a c t i v a t e d w i t h p r o b a b i l i t y T , one f i n d s
VN = NOIT ( 1 - T ) -N IT 0
PN = NOT
u, = P vx = p ( l - p )
Thus ,
!Js = NoTP
Vs = No'Tp(l-p) + NoTp2 = Norp
As a r e s u l t , t h e d i s t r i b u t i o n f o r t h e o v e r - a l l (compound)
process i s e q u i v a l e n t t o a s imple Poisson d i s t r i b u t i o n with
mean and va r i ance both e q u a l t o Nonp.
p r o b a b i l i t y of producing a count is high ( p z l ) , t h e sma l l
Thus, even when t h e
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INTERPRETATION OF ERRORS IN COUNTING EXPERIMENTS
r e a c t i o n p r o b a b i l i t y ( n < < l ) p r e se rves t h e Poisson c h a r a c t e r
of t h e p rocess . 7
S i m i l a r conclusions apply t o a l a r g e number of phys i ca l
experiments -- i n which one i s b a s i c a l l y i n t e r e s t e d i n t h e
i n i t i a l number of atoms, a r e a c t i o n c r o s s s e c t i o n , o r an
( a c t i v a t i n g ) p a r t i c l e f l u x . I t should be noted, i n pas s ing ,
t h a t o t h e r compound d i s t r i b u t i o n s do n o t l ead t o such simple
s o l u t i o n s as t h e above Poisson-Binomial combination. The
more gene ra l compound Poisson d i s t r i b u t i o n -- of concern i n
t h e fol lowing s e c t i o n -- has a va r i ance which exceeds t h e
mean, because t h e Poisson parameter i t s e l f i s randomly d i s t r i b
uted5 ' 6.
C H I - SQUARED AND WEIGHTED LEAST SQUARES
Weighted least squa res c a l c u l a t i o n s , which are commonly
used f o r f i t t i n g nuc lea r s p e c t r a o r decay curves, i nvo lve t h e
a p p l i c a t i o n of weights (wi) t o t h e obse rva t ions ( y . ) t o d e r i v e
a t e s t s t a t i s t i c , 1
2 - pi) / d . f .
which i s d i s t r i b u t e d as X2/d.f., provided t h a t t h e weights
G = C W . (y i i
are t h e i n v e r s e va r i ances . (d . f . r e p r e s e n t s t h e number of
degrees of freedom.) Comparison of G w i th i t s expected
va lue , u n i t y , p rov ides a d i s p e r s i o n t e s t of t h e f i t . On
t h e o t h e r hand, i f t h e weights are only p r o p o r t i o n a l t o t h e
i n v e r s e va r i ances , t hen G s e r v e s t o estimate t h e cons t an t of
p r o p o r t i o n a l i t y , and t h e s t a n d a r d e r r o r estimate must t hen
include t h e f a c t o r c. Confusion between t h e s e two uses f o r G r e s u l t s i n t h e
common mistake of mul t ip ly ing t h e s t a n d a r d e r r o r e s t i m a t e by
fi whenever G i s n o t w i t h i n accep tab le bounds. Except f o r
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L. A . CURRIE
t h e case where t h e var iances a re a l l underestimated by the
same f a c t o r , t h i s i s not a co r rec t procedure; it may prevent
t h e recogni t ion of i nco r rec t models or var iances and it may
lead t o wrong s tandard e r r o r es t imates .
--
A d e t a i l e d examination of t h i s problem has been given
elsewhere f o r an ac t iva t ion ana lys i s experiment involving
t h e more general compound Poisson d i s t r i b u t i o n , i n which
the index of d i spers ion exceeds uni ty . In t h i s experiment,
t h e variances d i f f e r e d from t h e simple Poisson values by an
add i t iona l (cons tan t ) var iance, a r a t h e r common s i t u a t i o n i n
8
r ad ioac t iv i ty measurements. Ignoring t h a t f a c t l ead t o a
"bad" f i t , but mu l t ip l i ca t ion of t h e s tandard e r r o r estimate
by fi did not y i e l d a co r rec t answer. The r e s u l t s of t h e
experiment -- t h e determination of oxygen by f a s t neutron
ac t iva t ion analysis ' -- appear i n Table 1. The f i r s t row
gives t h e (weighted) mean r a t i o of unknown t o s tandard (ne t )
c o u t s , based upon 10 observat ions, and t h e following rows
r e l a t e t o the respec t ive s tandard e r r o r s .
TABLE 1
Oxygen Act ivat ion Analysis -- Weighted
Mean Ratios and Standard Errors
Poisson Weights*
Mean Ratio 2 .006
Standard Error
(1) from weights 0 .o1g2
( 2 ) x a 0.0884
( 3 ) cor rec t value 0 . 1 4 9
True Weights
2 . 1 4 6
0 .119
-- --
2 -1 *wi =
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I N T E R P R E T A T I O N OF ERRORS I N COUNTING EXPERIMENTS
The r e s u l t of u s ing count ing s t a t i s t i c s on ly ("Poisson
Weights") -- 2 .006 - + 0.019 -- w a s accompanied by a value of
4 .60 f o r a, i n d i c a t i v e of a very poor f i t . Erroneously
mul t ip ly ing by fi produced t h e r e v i s e d s t anda rd error
e s t i m a t e 0.0884.
e r r o r of t h e r e s u l t 2 .006 i s 0 . 1 4 9 and it may be de r ived , as
shown i n r e f e r e n c e 8 , from t h e r a t i o s of t h e t r u e t o assumed
(Poisson) va r i ances .
However, t h e c o r r e c t value f o r t h e s t anda rd
A b e t t e r procedure i n t h i s case is t o inc lude t h e 2 a d d i t i o n a l va r i ance component (axs) i n t h e weights -- i . e .
w . = ( a + (I ) -' Then G serves a s a t es t s t a t i s t i c i f t h e 1 xs p i '
a d d i t i o n a l va r i ance component i s known, o r G may be se t e q u a l
t o i t s expected value ( u n i t y ) i n o r d e r t o estimate t h e
a d d i t i o n a l va r i ance . The c a l c u l a t i o n i s d i scussed i n some
d e t a i l i n r e f e r e n c e 8 , where it i s shown t h a t t h e best estimate
and i t s s t anda rd e r r o r i s 2 . 1 4 6 f 0.119. The r e s u l t of u s ing
j u s t Poisson weights , 2.006, i s accep tab le i n t h a t it i s
unbiased, b u t i t s va r i ance i s l a r g e r t han t h a t of t h e 2 . 1 4 6
estimate by a f a c t o r of about 1 . 6 . On t h e o t h e r hand, "cor-
r e c t i o n " by t h e f a c t o r fi l eads t o an e s t ima ted va r i ance ( f o r
2.006) which i s t o o small by a f a c t o r of about 2.8.
By way of summary, s t anda rd e r r o r m u l t i p l i c a t i o n by fi
should be used only i f r e l a t i v e weights (and va r i ances ) are
c o r r e c t l y known. The more common p h y s i c a l s i t u a t i o n i n which
t h e (assumed) va r i ances are underestimated because of a missing
e r r o r component r a t h e r t han by a common f a c t o r must be t r e a t e d
as d i s c u s s e d i n t h e preceding paragraph. Otherwise model
e r r o r s may go unrecognized, b e s t (minimum va r i ance ) estimates
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L. A. CURRIE
w i l l n o t r e s u l t , and s t a n d a r d e r r o r estimates w i l l be inco r - 10 rect .
POISSON DISPERSION TEST
A b r i e f remark about L e x i s ' d i s p e r s i o n t e s t f o r Poisson
v a r i a b l e s may prove h e l p f u l i n exposing ano the r p o t e n t i a l
source of confusion i n coun t ing experiments . I n t h i s t e s t ,
t h e sum of t h e squa res of t h e d e v i a t i o n s of n-repeated counts
(xi) from t h e mean va lue (x) is d i v i d e d by t h e mean value:
- X
1 2 2 2
X / d . f . a sympto t i ca l ly approaches t h e v a r i a n c e r a t i o s /a ,
and t h e r e f o r e it has approximately t h e X2/d.f. d i s t r i b u t i o n .
Th i s r e s u l t , i n which d . f . = n-1, i s t r e a t e d i n some d e t a i l by
Cox and Lewis".
D i f f i c u l t i e s may a r i s e , however, when one compares
t h i s d i s p e r s i o n t e s t with Pea r son ' s x 2 t e s t f o r goodness-
o f - f i t u s ing c - c l a s s e s of d a t a . I n t h i s case where one
examines t h e frequency of occurrence ( f . ) f o r d i f f e r e n t
c l a s s e s (magnitudes) of counts r a t h e r t han t h e counts them-
s e l v e s , t h e number of degrees of freedom i s c-1-PI where P
e q u a l s t h e number of parameters e s t i m a t e d from t h e d a t a . (As
t h e c-classes cover t h e e n t i r e sample space , t h e number of
independent f r equenc ie s cannot exceed c-1) . Thus, count ing
(Poisson) experiments , i n which t h e mean i s e s t i m a t e d from
t h e d a t a , y i e l d c-2 degrees of freedom.
3
Confusion d i sappea r s immediately i f one recognizes t h e
f a c t t h a t t h e r e are two d i f f e r e n t tests invo lved , one f o r
d i s p e r s i o n and one f o r goodness -o f - f i t f o r grouped observa-
t i o n s . B o t h tests a r e c a r r i e d o u t with t h e x2 s t a t i s t i c ,
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INTERPRETATION OF ERRORS IN COUNTING EXPERIMENTS
and, f o r Poisson v a r i a b l e s , t h e two tes t s formally look
very much a l i k e . Th i s formal s i m i l a r i t y , i n f a c t , goes
deeper , €or i n t h e goodness-of-f i t t e s t ( f o r any assumed
d i s t r i b u t i o n ) t h e obse rva t ions i n each class may be considered
t o fo l low independent Poisson d i s t r i b u t i o n s 1 2 -- a f a c t
which i n c i d e n t a l l y i s h e l p f u l i n dec id ing upon t h e minimum
accep tab le frequency p e r class i n t e r v a l .
In g e n e r a l it would seem d e s i r a b l e t o use t h e d i s p e r s i o n
t e s t ( d . f . = n-1) r a t h e r t han t h e goodness-of-€it (class)
t e s t ( d . f . = c-2) f o r Poisson va r i ab le s13 .
tes t , which g e n e r a l l y has many more degrees of freedom, f r e -
quen t ly proves t h e more s e n s i t i v e . A d e t a i l e d and very il-
luminat ing d i s c u s s i o n of t h e e n t i r e problem has been given
by Cochran .
The d i s p e r s i o n
1 2
ACKNOWLEDGMENT
The au tho r i s most g r a t e f u l f o r t h e s t i m u l a t i n g d i scus -
s i o n s and t h e h o s p i t a l i t y of P ro f . H. Oeschger and h i s co l -
leagues of t h e Phys ika l i s ches I n s t i t u t d e r U n i v e r s i t a t Bern,
where t h i s work was c a r r i e d o u t . Helpful d i s c u s s i o n s a l s o
took p l a c e with D r . H. Riedwyl, D r . S t r e i t and P ro f . A. N i r .
P a r t i a l suppor t from t h e “Schweizer ischer Nat ionalfonds” i s
g r a t e f u l l y acknowledged.
1.
2.
3.
4 .
EFEENCES
G. F r i ed lande r , J. W. sennedy, and J. M. M i l l e r , Nuclear and Radiochemistry, 2n E d i t . , Wiley ( N e w York) 1 9 6 4 .
P. C. J u r s and T. L. Isenhour , Anal. Chem. - 39 1388 (1967) .
The d i f f i c u l t y becomes obvious if p+l. Then t h e assumed variance e q u a l s ze ro , even though N i s a random v a r i a b l e .
P. C. Stevenson, ‘Processing of Counting Data ,” NAS-NS- 3109 ( 1 9 6 6 ) .
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L. A. CURRIE
5.
6 .
7.
8 .
9 .
10.
11.
1 2 .
13.
W. F e l l e r , An I n t r o d u c t i o n t o P r o b a b i l i t y Theory and Its A p p l i c a t i o n s , 2nd E d i t . , V o l . I , Chapt . X I I , Wiley ( N e w York) 1957.
J. Byrne, P h y s i c a - 41 575 (1969) .
The Binomial e x p r e s s i o n f o r t h e v a r i a n c e , Np(1-p) , may be of use i n o p t i m i z i n g t h e l a s t s t e p ( c o u n t i n g ) of t h e compound p r o c e s s , b u t one must be aware of t h e p o s s i b i l i t y o f c o r r e l a t i o n i f s e q u e n t i a l c o u n t i n g t i m e s are invo lved .
L. A. C u r r i e , "The L i m i t of P r e c i s i o n i n Nuc lea r and A n a l y t i c a l Chemis t ry" , s u b m i t t e d t o Nucl. I n s t . Meth.
F. A. Lundgren and S. S. Nargo lwa l l a , Anal. Chem. - 40 672 (1968) .
One o f t h e few r e p o r t e d cases where t h e l i m i t a t i o n s o f u s i n g fi as a scale f a c t o r h a s been r ecogn ized is i n t h e c o n t i n u i n g review of Fundamental P a r t i c l e P r o p e r t i e s by t h e P a r t i c l e D a t a Group (A. Barbaro-Galtieri , S. E. Derenzo, L. R. P r i c e , A. R i t t e n b e r t , A. H. Rosenfe ld , N. Barash- Schmidt , C. Bricman, M. ROOS, P. Soding and C. G. Wohl, Rev. Mod. Phys. 42 87 ( 1 9 7 0 ) ) . Even h e r e , however, it would seem l i k e l y t h a t t h e a d d i t i o n a l v a r i a n c e component approach might l e a d t o a more reliable and more c o n s e r v a t i v e estimate f o r t h e s t a n d a r d error as w e l l as a more p r e c i s e estimate f o r t h e mean of t h e p a r t i c l e p r o p e r t y i n ques- t i o n .
D. R. Cox and P. A. W. L e w i s , The S t a t i s t i c a l Ana lys i s of Series of Even t s , Chapt . 6 , Wiley (1966) .
W. G. Cochran, Ann. Math. S t a t . 23 315 (1952) .
d . f . is h e r e g i v e n f o r t h e case where x is de te rmined from t h e o b s e r v a t i o n s . If a known mean i s assumed, d . f . f o r t h e t w o tests become n , and c-1, r e s p e c t i v e l y . The "miss ing" d . f . i s due t o t h e s i n g l e l i n e a r c o n s t r a i n t , Cf. = n, whereas t h e r e are no c o n s t r a i n t s among t h e
-
Xi. I
Rece ived October 1 3 , 1971
Accepted October 18 , 1971
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