In 1944, not only were there uncer-
tainties in the animal data, but meth-
ods for measuring the amount of plu-
tonium retained in the bodies of
workers were not well defined. Peo-
ple realized that because plutonium
was an alpha emitter, the radiation
was readily absorbed by the sur-
rounding material, and analysis of
excreta for plutonium activity offered
the most promising route for estimat-
ing body burdens of internal plutoni-
um. However, the low excretion
rates predicted from animal experi-
ments would make analysis difficult.
On the first day after injection, when
the fecal and urinary excretion rates
were at their highest, the total amount
excreted in the urine in 24 hours was
less than 10 per cent of the amount
injected, and similarly with feces.
The excretion rates then dropped
rapidly for several weeks, finally lev-
eling off, for urine, at only 0.01 per
cent of the injected plutonium.
Although large doses could be inject-
ed into animals to insure good analyt-
ical results, the same could not be
done with humans. If an 0.01-per-
cent daily urinary excretion rate was
true for humans, a 24-hour urine
sample from a subject with 5 micro-
grams of retained plutonium would
contain only 0.5 nanograms (nano =
10
-9
) of plutonium (see “Estimates of
the Detection Regime”).
Excreta samples also had the problem
that most of the alpha radiation
would be absorbed by the sample
mass. Thus, analytical techniques
had to be developed to reduce the
mass of other material and to concen-
trate the plutonium by dissolving,
evaporating, or ashing the sample and
by extracting, precipitating, or plating
the plutonium for measurement of
alpha activity.
Ion-exchange. That summer, the
Met Lab’s Health Division developed
a urinalysis procedure for isolating
and detecting tenths of nanograms of
plutonium in urine. The method was
based on direct isolation of the pluto-
nium by passing an acidified 100-mil-
liliter urine sample through a cation-
exchange resin. After the resin had
captured the plutonium, the concen-
trated metal was eluted from the col-
umn and transferred to a counting
plate where the alpha activity was
measured.
In July 1944, Hempelmann was in-
formed of the Met Lab urinalysis
procedure and of the apparent con-
stant 0.01 per cent urinary excretion
rate derived from animal studies.
Several items—such as his calcula-
tion for the dose to the lungs from a
1-microgram plutonium dust particle,
early results from the animal experi-
ments, and a difference of opinion of
a factor of 10 about what constituted
a “safe” alpha radiation dose for tis-
sue cells—were beginning to make
him think that detection methods
needed to be sensitive to lower levels
than the proposed 5-microgram toler-
ance limit. Also, the Met Lab had
determined that blood counts gave
evidence of over-dosage but not until
a relatively late stage following depo-
sition of the plutonium in the bone.
Thus, Hempelmann informed Oppen-
heimer that analysis of excreta sam-
ples in the early stages following ex-
posure, when the excretion rates were
highest, was the only method for
early detection of overexposure.
Hempelmann assigned a biochemist,
Anne Perley, to investigate if the
Chicago procedure was suitable for
detecting 1-microgram body burdens.
By the end of the month, she in-
formed him that the combination of
the Met Lab procedure and the Los
Alamos alpha counters were inade-
quate for detection of plutonium lev-
els consistent with 1-microgram body
burdens. In fact, attempts to use the
The Human Plutonium Injection Experiments
Number 23 1995
Los Alamos Science
191
Detection of Internal Plutonium
the program that he, Warren, Kennedy,
and Oppenheimer had decided upon.
Los Alamos would develop “chemical
methods of determining plutonium in
the excreta and in tissues and of ioniza-
tion methods of detecting plutonium in
the lungs.” Experiments at Los Alamos
with animals would be used to check
the detection methods. The third part
of the program would involve “tracer
experiments on humans to determine
the percentage of plutonium excreted
daily.”
It was stated that “when satisfactory an-
alytical methods have been developed
in this laboratory the problem of carry-
ing out further metabolic studies will be
turned over to another medical group,
presumably the Rochester group.” Ini-
tially, Rochester would determine the
lethal dose in animals using plutonium
supplied by Los Alamos.
The excretion rate. By February
1945, Los Alamos, the Met Lab, and
the Berkeley groups all had analytical
methods they felt were adequate for the
analysis of plutonium in excreta (see
“Detection of Internal Plutonium”).
They could thus turn to the next puzzle,
the ratio of excreted to retained plutoni-
um. Much of the animal data showed
that a constant daily urinary excretion
rate occurred within two or three weeks
that was 0.01 per cent of the initial in-
jection. By March, urine samples from
Los Alamos workers were indicating,
based on the 0.01-per-cent rate, that
some of the workers were approaching
or had exceeded a body burden of one
microgram. Concern about this situa-
tion was mounting.
There were other discrepancies and
concerns. Numerous workers with high
nose-swipe counts had no definite sign
of plutonium in their urine. Was this
due to hand contamination of the nose,
insoluble plutonium particles that had
not reached the circulatory sytem, or
large particles still lodged in the upper
bronchi and nasal passages? The large
variations in the animal data for the uri-
continued on page 194