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Overview of Transuranium Elements

Notes for msc chemistry first sem nuclear chemistry

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0% found this document useful (0 votes)
59 views24 pages

Overview of Transuranium Elements

Notes for msc chemistry first sem nuclear chemistry

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Akhil Binu
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© All Rights Reserved
We take content rights seriously. If you suspect this is your content, claim it here.
Available Formats
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UCRL-JC-124728

(La/if- 9 0 07/29 ~-3

The Transuranium Elements:


From Neptunium and Plutonium
to Element 112

Professor Darleane C. Hoffman


Lawrence Livermore National Laboratory
G. T. Seaborg Institute for Transactinium Science
Isotope Sciences Division
SEP 2 3 896

This paper was prepared for submittal to the


Conference Proceedings
NATO Advanced Study Institute on "Actinides and the Environment"
Chania, Crete, Greece
July 7-19, 1996

July 26, 1996

1
LL6421#v1.0(3ra6) atSTRiBUTION OF THIS DOCUMENT IS UNLIMITED
DISCLAIMER
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the United States Government. Neither the United States Government nor the
University of California nor any of their employees, makes any warranty, express
or implied, or assumes any legal liability or responsibility for the accuracy,
completeness, or usefulness of any information, apparatus, product, or process
disclosed, or represents that its use would not infringe privately owned rights.
Reference herein to any specific commercial product, process, or service by trade
name, trademark, manufacturer, or otherwise, does not necessarily constitute or
imply its endorsement, recommendation, or favoring by the United States
Government or the University of California. The views and opinions of authors
expressed herein do not necessarily state or reflect those of the United States
Government or the University of California, and shall not be used for advertising
or product endorsement purposes.
DISCLAIMER

Portions of this document may be illegible


in electronic image products. Images are
produced from the best available original
document.
THE TRANSURANIUM ELEMENTS:
FROM NEPTUNIUM AND PLUTONIUM TO ELEMENT 112

Darleane C. Hoffman
Nuclear Science Division & Chemistry Department, University of
California, Berkeley, CA 94720 & G. T. Seaborg Institute for
Transactinium Science, MS-L231, LLNL, Livermore, CA 94550.

1. Introduction

Beginning in the mid-1930's, spurred by the discovery of the neutron by Chadwick in


1932 and artificial radioactivity by the Joliot-Curies in 1934, the new breed of nuclear
scientists (including both chemists and physicists) became intrigued with the prospect of
synthesizing new "artificial" elements not found in nature. Uranium, the heaviest
known element, had been discovered in 1789 and yet it was to be nearly 150 years
before the ancient alchemists' dream of transmutation was achieved with the synthesis of
the first transuranium element, neptunium, in 1940. Over the past six decades, 20
transuranium elements have been produced. (See Figure 1 which shows the current
periodic table as of mid-1996). .

2. Nuclear Fission

Inextricably intertwined with the discovery of transuranium elements has been the
discovery and study of nuclear fission. Fermi and coworkers began experiments in
1934 to try to produce element 93 by bombarding uranium with neutrons to give 239TJ
which they expected would beta decay to produce "S>93. Based on the then accepted
periodic table, they believed element 93 should behave like the lighter homologs
manganese and rhenium (see Figure 2 which shows periodic table from before World
War II). They performed a chemical separation designed to separate element 93 with a
precipitate of rhenium sulfide and found a 13-minute activity which in a paper published
in 1934 [1] they tentatively assigned to element 93. Ida Noddack (a discoverer of
rhenium ) published a paper [2] soon after in which she expressed her doubt about their
assignment and suggested that the bombarded nuclei might have disintegrated into
several larger fragments! In subsequent years, Hahn, Meitner, and Strassmann [3] in
Berlin seemed to confirm these results and reported other isotopes of eka-rhenium as
well as of eka-osmium, -iridium, and -platinum. However, there were many unsettling
aspects about these results and in 1938 Curie and Savitch [4] found a 3.5-hour activity
with the chemical properties of a rare earth, but they were unable to explain this and it
was at first greeted with some skepticism by the Berlin group. Finally, Hahn and
Strassmann decided to perform their own experiments and found several new activities
which they attributed to radium and actinium istopes and isomers. Meitner (now in
Stockholm) at least, found these results unsatisfying: there were now some 16 new
species that originated with " O J J , including multiple isomerism, and beta-decay
energies which were too high for the measured half-lives! Furthermore, the yields were
markedly enhanced when slow neutrons were used, making the postulated (n, a)
reactions to make thorium which then cc-decayed to Ra (Ac) isotopes energetically
impossible. Meitner urged that they re-examine the experiments and it was then that
Hahn and Strassmann [5] began the series of experiments which culminated in the
discovery of nuclear fission by showing that the activities attributed to Ra, Ac, and Th
actually followed the chemistry of Ba, La, and Ce!! But they still hesitated to believe
their results, and stated, "As nuclear chemists, being in some respects close to physics,
we have not yet been able to take this leap which contradicts all previous experiences in
nuclear physics. It could still perhaps be that a series of unusual coincidences have
given us deceptive results."
However, during the Christmas holidays of 1938, Meitner together with her
nephew, physicist Otto Robert Frisch, who had come to visit her in Sweden, unraveled
the puzzle. They worked out all the essential features of nuclear fission based on the
liquid drop model and the masses involved. Upon returning to Copenhagen, Frisch
spoke with Niels Bohr who immediately agreed with their interpretation and they
proceeded to submit a letter to Nature on "Disintegration of Uranium by Neutrons: A
New Type of Nuclear Reaction" [6]. In this elegant paper, in just over a page, they
outlined the essentials of the theory of nuclear fission, including the total energy
released and the recoil energy of the fission fragments, which Frisch [7] quickly
detected experimentally .

3. The Actinide Elements

3.1 NEPTUNIUM (93) AND PLUTONIUM (94)

Now there were no more transuranium elements, as Fermi's transuranium elements


could all be attributed to fission products which had obscured the activity of the new
element 93. Seemingly, all of the nuclear scientists in the world then set out to
investigate the new phenomenon and in Berkeley, Edwin M. McMillan, while
investigating the recoil of fission products produced in the irradiation of a thin layer of
23<>u with slow neutrons, found a 2.3-day activity which did not recoil out and
appeared to be the daughter of 23-minute 2 3 % . In the spring of 1940 he and Philip H.
Abelson chemically separated and identified [8] the new element Np.

238TJ + n > 239TJ + r> 239TJ p. 23 minutes-, 2 3 9 N p p. 2.3 d > 239 9 4

It was obvious to them that the new element should beta decay to the same mass number
of element 94, but they were unable to identify it. Bombardments were begun with
deuterons in the 60-Inch Cyclotron at Berkeley, but McMillan was called away and
Glenn T. Seaborg wrote to ask him whether he and his graduate student Arthur C. Wahl
and a fellow instructor Joseph W. Kennedy should carry on this research. He agreed
and in December 1940 they detected alpha decay of an activity which grew in to the
ehemically separated neptunium fraction and had a half-life estimated to be about 50
years.

238rj + 2 H >238Np + 2 n; 238 N p _ f i _ > 2 3 8 p u (-50 years)

They sent a short note to Washington describing their results, but didn't consider they
had sufficient proof to claim discovery until finally on the night of February 23, 1941,
Art Wahl oxidized it with peroxydisulphate + Ag + * and it was shown to have
properties similar to U but not to Os as suggested earlier. This was also communicated
to Washington, but these two articles were not published until 1946 [9,10]. Soon after,
a 1.2 kg sample of uranyl nitrate was irradiated with neutrons in the 60-Inch Cyclotron
for two days in order to produce enough 2 3 ^Np so that after its purification it would
decay to form 0.5 \ig of 239p u w } , o s e half-life was calculated to be about 30,000
years. Shortly after in March, 1941, it was shown that its fission cross section with
slow neutrons was about 50% greater than for •"-'U, which was later published by
Kennedy, Seaborg, Segre, and Wahl [11]. This information formed the basis for the U.
S. wartime Plutonium Project at the Metallurgical Laboratory of the University of
Chicago whose mission was to develop a method for the production of Pu in quantity
and for its chemical separation on a large scale.
Elements 93 and 94 were named neptunium (Np) and plutonium (Pu), because
uranium was originally named after Uranus, and Neptune and Pluto are the next planets
beyond Uranus, hence, the names neptunium and plutonium. (For more details on these
discoveries and naming, see G. T. Seaborg, [12].)

3.2. AMERICIUM (95) THROUGH FERMIUM(IOO)

All of these elements were produced first either via neutron or helium-ion
bombardments in the years between 1944 and 1955. Initially, unsuccessful attempts
were made to produce and chemically separate elements 95 and 96 believing that they
were part of a uranide series with U as the prototype and would have chemical
properties similar to Pu, Np, and U. Finally, in 1944 Seaborg proposed in an article
published later in Chemical & Engineering News [13] that maybe this new series should
start at thorium with actinium as the prototype, as shown in Figure 3. Then elements 95
and 96 might have properties similar to Eu and Gd and, therefore, could be oxidized
beyond the III state only with great difficulty. Element 96 was produced [13] in 1944
via the 239p u ( a> n ) 242pg reaction at the Berkeley 60-Inch Cyclotron and was
shipped to the Met Lab for processing. In 1945, 24195 Was produced by A. Ghiorso ex
al. [14] by multiple neutron capture in -"9p u bombarded in a reactor. The names
americium and curium were proposed for elements 95 and 96 by analogy to europium
and gadolinium which were named after Europe and after Johan Gadolin, a Finnish rare-
earth chemist. These two elements were exceedingly difficult to separate from each
other until the development of ion-exchange techniques which were also to be widely
used in the separation of subsequent actinides.
Next came the discovery of berkelium (97) in 1949 produced via the 241 Am (a,
2n) 2 4 3 9 7 (4.5 h) reaction [15] and californium (98) produced [16] via the 2 4 2 C m (a,
n) 2 4 ^98 (44 mjn) rea ction at the Berkeley 60-Inch Cyclotron. Key to discovery of Bk
was removal of the large amount of Am target material by oxidizing it to the
hexapositive state and subsequent elution of the Bk from a cation exchange column just
ahead of Cm. The californium (98) experiment used a few micrograms of the highly
radioactive target 2 42c! m and the identification of Cf was made with a total of only
about 5,000 atoms using elution from a cation exchange resin column to identify it. The
names berkelium and californium were chosen to honor the city and state of discovery.
Although most of the discoveries of the transuranium elements were carefully
planned based on the best available knowledge concerning chemical and nuclear
properties, elements 99 and 100 were synthesized in a most dramatic, unplanned, and
unexpected manner in the first U. S. thermonuclear device "Mike" tested at Eniwetok
in November, 1952. Because of the enormous, nearly instantaneous high neutron flux
generated in its detonation (see Figure 4) at least 17 neutrons were successively
captured in the 23°U to produce isotopes through 2 ^ U . In subsequent tests, 257p m
was detected, indicating capture of at least 19 neutrons! These short-lived uranium
isotopes then beta-decayed to the more stable, higher Z elements as shown in Figure 5.
Early analyses at Los Alamos Scientific Laboratory and Argonne National Laboratory
to determine the performance of the test showed the first evidence that something truly
unexpected had occurred when the new very neutron-rich isotopes 2 44p u (-80 million
years, still the longest known isotope of Pu) was found in mass spectrometric analyses,
and 246p u (i i d) w a s found in Pu samples separated from the debris collected after the
test. This led the Berkeley group to join the other two Labs in a search for trans-Cf
isotopes. Eventually tons of coral were laboriously processed and the 20-day 25399
and 20-h 255 JQQ w e r e positively identified using the technique of elution from a cation-
exchange resin column. Although this "discovery" was unplanned, the previous
experience with the ion exchange elution technique, the prediction that Es and Fm
should be +3's, and their predicted elution positions based on their positions in the
actinide series, were instrumental in the discoveries. After much discussion, the names
einsteinium (Es) and fermium (Fm), after the great scientists Albert Einstein and Enrico
Fermi, were chosen for these elements. (It should be noted that Einstein and Fermi
were both still alive when these names were proposed.) After later declassification, the
discovery of Es and Fm was published in 1955 [17]. Although subsequent attempts were
made to produce still heavier elements in underground nuclear tests, 257Fm was the
heaviest isotope which could be synthesized and detected using neutron-capture
reactions. (See Figure 5.)

3.3. THE END OF THE ACTINIDES: MENDELEVIUM (101) THROUGH


LAWRENCIUM(103)

Element 101 is the first element which was produced and identified an "atom-at-a-time"
using a target of only about 10^ atoms of 253g s produced by irradiation of Pu in the
Materials Testing Reactor. The (a,n) reaction at the 60-Inch Cyclotron was used [18] in
1955 to make —^^ 101. For the first time in this type of experiment, the "recoil"
technique in which the reaction products recoiling out of the very thin target are
collected on a "catcher" foil. The foil is then quickly removed and chemically
processed without destroying the very precious target so it can be used over and over
again. Only about one atom per irradiation was expected. The ion exchange method
with alpha-hyroxyisobutyrate as eluant was used and 5 spontaneous fissions (SFs) were
observed in the 101 position and 8 in the 100 position. From the half-lives and other
evidence it was established that ^ " 1 0 1 decays by electron capture to 25"\QQ which
then decays by SF. The name mendelevium was suggested in honor of Dimitri
Mendeleev, the great Russian chemist who formulated and pioneered the use of the
periodic table of the elements to predict chemical properties of unknown elements.
The discovery of element 102 was first reported in 1957 by an international group
[19] of scientists from Argonne National Laboratory in the U. S., the Atomic Energy
Research Establishment in Harwell, England and the Nobel Institute of Physics in
Stockholm. They irradiated a 244cm target with ^ C ions at the Cyclotron at the Nobel
Institute and detected a 10-minute activity which decayed via 8.5-MeV alpha emission,
which they attributed to element 102. The assignment was based on its elution from an
ion-exchange column with alpha-hydroxyisobutyrate in the expected position for
element 102, i.e., just after the free column volume and they suggested the name
nobelium in honor of Alfred Nobel. Researchers at both Berkeley [20] and the
Kurchatov Institute in Moscow [21] were unable to confirm this result and much later
experiments at Berkeley [22] showed that, in fact, the most stable oxidation state of
element 102 in aqueous solution was 2 + and, therefore, would not have eluted in the
position expected for a trivalent actinide. For a more complete review of the chemistry
of the chemistry of the elements heavier than fermium (100), see Refs. 23 and 24.
Experiments at Berkeley in 1958 by Ghiorso et al. [25] identified 2 5 4 102 (55 s) in the
reaction of Cm with ^C ions based on chemical identification of its 254 JQ2 (30
min) daughter activity. In direct counting in recoil experiments, a 3-s half-life was
erroneously assigned to this isotope, but it was later found to be due to ^52 JQ2 (2.3 s)
produced from 2 4 4 C m in the target. In 1958 in the reaction of 2 3 9 P u with ^ O ions,
Flerov et al. [26] at the Kurchatov Institute reported producing an 8.9-MeV alpha-
emitter with a 2 to 40 s half-life which they attributed to 102. Later (1964) Donets et al.
[27] produced 2 ^"102 and chemically identified its 252p m daughter. Subsequently, at
Dubna, the correct measurement of the half-life of 2 ^ 4 102 was made. Thus, credit for
discovery of element 102 was really shared by the Berkeley group and Donets et a!, at
Dubna. Since the name nobelium (No) was already in common use, the Berkeley group
suggested that this name be retained.
Element 103 was first produced and identified at the Berkeley HILAC in 1961 by
Ghiorso et al.. [28] in the following reaction:

249-252 Cf ( 10.1 l B x n ) 257,258 103 ( L r ) 8,6,MeV a, ,8 s ^

The recoiling atoms were caught on metalized Mylar tape which was moved past a
series of alpha detectors which recorded activity from a few new 257,_o8jo3 nuclei
with half-lives of seconds or less. They suggested the name lawrencium after E. O.
Lawrence, the inventor of the cyclotron and the founder of the Berkeley Radiation
Laboratory. The name was accepted by IUPAC, but the original symbol of Lw was
changed to Lr.
Later, Donets et al. [29] in 1965 used a double-recoil technique to positively
identify the atomic number of element 103 by linking its decay, via either electron
capture (ec) followed by alpha decay, or by alpha decay followed by ec, to its known
granddaughter, 252p m> ^vhich decays with a half-life of 25 hours. This daughter was
identified both chemically and by its characteristic alpha decay. Thus, some credit for
discovery of element 103 should be shared by Donets et al
243
Arn( 1 8 O,5n) 2 5 6 Lr ^ ~ 4 5 s
> 252 Md(101) ec 2m
i > 2 5 2 F m (known)

Figure 6 shows all the currently known isotopes of Lr and the heavier elements. In
1970, Silva et al. [30] used the 26-s 2 ^ L r to perform chemical studies which
established that the most stable oxidation state of Lr in aqueous solution is 3+, as
expected from Seaborg's actinide hypothesis, which also predicted that with filling of
the 5f shell Lr should end the actinide series.

4. The Transactinide Elements

4.1. RUTHERFORDIUM (ELEMENT 104) THROUGH SEABORGIUM


(ELEMENT 106)

4.1.1. Rutherfordium (Element 104)


Controversy has surrounded the discovery of elements 104 and 105 ever since the very
first reports; for a comprehensive discussion of the claims and counterclaims and a
bibliography of all the published literature, see Hyde, Hoffman, and Keller [31]. In
1964, Flerov et al. [32] reported detection of a 0.3-s spontaneously fissioning activity
produced at the heavy ion cyclotron at the Joint Institutes of Nuclear Research (JINR)
at Dubna in the following reaction:
242
Pu( 2 2 Ne, 4n ) 2 6 0 104 (o~0.2 nb) S F - °- 3 s >(58 SFs)

Recoils were collected on a nickel conveyer belt which was moved past special
phosphate glass detectors where the fission events were recorded. From the distribution
of etched tracks and the known speed of the belt the half-life could be deduced. The
bombarding energy of the Ne projectiles was also varied and the excitation function
indicated that a 4n reaction had been observed.
However, one of the problems involved in claiming discovery of a new element
only by observation of its SF activity is the difficulty of proving the atomic number of
the fissioning species since the fission process effectively destroys this. Consequently,
in an effort to confirm the atomic number of this SF activity, gas chromatographic
separations were performed over the years 1966-69 by Zvara et al. [33]. They based
their separation on the actinide hypothesis which predicted that element 104 should be
eka-hafnium and tried to show that the 0.3-s SF activity had a volatile chloride and
would follow the volatile HfCl4 while the heavy actinides would not. These
experiments used isothermal chromatography (250 or 300 °C and were designed for a
half-life of 0.3 s. (Possible contamination from Pu was recognized as a potential
problem.) A total of 14 SFs were recorded in mica detectors in this series of
experiments and attributed to 2 °0l04. The authors stated that the fission track
distribution was consistent with a 0.3-s half-life and "shows positively that the effect
was not caused to an appreciable extent by the decay of nuclides undergoing SF with
half-lives of 0.014 s and 3.7 s". Later experiments reported by Zvara et al. in 1969-
1970 [34] were in agreement with the previous ones and they accepted 0.5 s as the
correct value of the SF half-life. (In 1969, Drain and coworkers determined the half-
life to be 0.1 s and subsequently it was dropped to 0.02 s, much too short to have been
observed in this chemistry!) However, the use of gas chromatography has since become
a valuable tool for studying chemical properties of the transactinide elements [23, 24].
Ghiorso et al. [35] in 1969 at the HILAC at LBL were unable to confirm existence
of a 0.3-s isotope of 2 6 0 104 using the reactions 246 Crn( 18 O,4n) and 248 Crn( 16 O,4n).
However, they chose to try to positively identify the Z and A of new a-emitting
isotopes of 104 using the method of a-a correlations in which the cc-decay of known
recoiling daughter activities is correlated with that of the parent. A new instrument
called the Vertical Wheel (VW) was developed for this purpose. The VW and the
following reactions were used to positively identify two new isotopes of element 104
[36]:

249
C f ( 12 C,4n) 257 104(Rf) (a-0.01 ub) a - ~ 4 - 5 s > 2 5 3 No (1.7 m)
249
C f ( 13 C,3n) 259 104(Rf) (CT-0.01 ub) ^^^^ ~ 3 s > > 2 5 5 No (3.1 m)
248
Crn( 1 6 O,5n) 2 5 9 104(Rf)

In 1973, an independent group of American scientists led by C. L. Bemis, Jr. [37] at


Oak Ridge National Laboratory confirmed the identification of • " ' 104 using the same
reaction as did Ghiorso et al. They identified the characteristic K X-rays of element
102 in coincidence with the a-particles from decay of the 4.5-s 2 ^^104.
The Berkeley group chose Rutherfordium, symbol Rf, for element 104 while the
Dubna group proposed Kurchatovium, symbol Ku. Rutherfordium (Rf) was accepted
by the American Chemical Society (ACS) in 1994 for use in their journals.

4.1.2. Hahnium (Element 105)


Flerov et al. reported in 1970 [38] that they had produced a 0.1- to 0.3-s cc-emitter at the
300-cm Cyclotron at Dubna in the following reaction:
243
A m ( 22 Ne, 5n ) 2 6 0 105 (0-0.1 n b )9.7-MeVa.0.1-3s >

The atoms recoiling out of the target were transported via He jet through an annular
detector to a metal collector wheel and correlations with a-daughter activities were
looked for. (A new apparatus was used for this purpose.) Unfortunately, the quality of
the alpha data is poor and even in 1971 papers by Druin et al. [39] shows no close
resemblance to the much better data published about the same time or even earlier by
Ghiorso et al. [40]. Zvara et al. again reported (unpublished results in 1970 and 1973)
using gas chromatography to attribute a 1.8-s SF activity reported earlier by Flerov et
al. to element 105, but from these results it is not possible to conclude that the observed
SFs are from a homolog of Nb and Ta, and hence, to element 105.
In papers published in 1970 [40] and 1971 [41], Ghiorso et al. presented
convincing evidence that isotopes of element 105 were produced and positively
• identified using the cc—a correlation technique with the VW in the following reactions
performed at the HILAC at Berkeley:

249
Cf( 1 5 N,4n) 2 6 0 105(Ha)(a-0.01^b)iJ^leVa 1 L6s > 2 5 6 L r (known 8.4-MeVa,30s)
25O
Cf( 1 5 N,4n) 2 6 1 105 8.93-MeV« 1 1.8s > 257 L r ^ Q65s}
249 18 262
Bk( O,5n) 105 8.45,8.66-MeVa, 40s ^ u (a> 3 9 s }

These results were later confirmed by Bemis et al. [42], using an L X-ray-alpha
coincidence technique.
The Berkeley group chose the name Hahnium, Ha, for element 105 and the Dubna
group proposed Nielsbohrium, Ns. Again, Hahnium (Ha) was approved by the ACS.
In 1974, an ad hoc committee of neutral experts was set up by the International
Union of Pure and Applied Chemistry (IUPAC) and the International Union of Pure and
Applied Physics (IUPAP) which included three members each from the USSR, the
USA, and three neutral countries. Their charter was "to consider the claims of priority
of discovery of elements 104 and 105 and to urge the laboratories at Berkeley and
Dubna to exchange representatives and in their presence to repeat the experiments
regarding these elements." However, these attempts proved fruitless and the committee
was disbanded. However, the American members decided to prepare and later publish
an article giving the history and an analysis of the discovery of elements 104 and 105
with a complete review of the experimental studies carried out at both laboratories
between 1960 to 1977, including a complete bibliography [31].

4.1.3. Seaborgium (Element 106)


Element 106 was produced by a Berkeley-Livermore group led by A. Ghiorso [43]
using the following reaction and the VW to measure a - a correlations with its known
a-emitting daughter, 3.0-s 25^Rf:

249
Cf ( 18 O,4n ) 263 106(a~0.6 nb) a. 0.9s > 2 5 9 R f a . 3 . Q S >

Recently, Gregorich et al. [44] confirmed the original experiment using a different
detection system and the 88-Inch Cyclotron at Lawrence Berkeley National Laboratory.
The name Seaborgium, symbol Sg, was proposed on behalf of the discovery group by
E. K. Hulet [45] at the April, 1994 National meeting of the American Chemical Society
(ACS). A short time later, Seaborgium (Sg) was approved by the ACS for use in its
journals.

4.2. NffiLSBOHRIUM(ELEMENT 107) THROUGH MEITNERIUM (ELEMENT


109)

Elements 101 through 106 were first produced using compound nucleus reactions
between actinide targets and light heavy ions in what might be called "hot fusion"
reactions because of the rather high excitation energy of the compound nucleus which
is produced. This increases the tendency for the compound system to fission promptly,
which results in lower and lower cross sections for the desired (xn) reactions, as the Z
of the compound nucleus is increased. It was suggested by Oganessian of Dubna that
"cold fusion" reactions between target nuclides near the doubly magic ^Oop^ (Z=^2,
N=152) might be used with appropriate neutron-rich heavy ion projectiles in the region
around Fe (26) to give a relatively "cold" compound system which might emit only 1 or
2 neutrons and have a much lower prompt fission cross section. A group at the
Gesellschaft fur Schwerionenforschung (GSI) in Darmstadt, Germany led by P.
Armbruster [46] exploited this type of reaction to produce the new elements 107, 108,
and 109. Their recently constructed Separator for Heavy Ion reaction Products (SHIP)
was used to separate the resulting reaction products from the beam projectiles and
identify the new element isotopes by measuring their decay chains to known daughter,
granddaughter, etc., nuclides.
In this way, positive identification of the new element isotopes could be made on
the basis of the observation of only a few atoms. The new elements 107, 108, and 109
were first identified [47, 48, 49] in the following reactions at the UNILAC at GSI,
Darmstadt:

209
Bi( 5 4 Cr,n) 2 6 2 107 (a -0.2 nb) 10-38-MeV a, -4.7 ms > k n o w n decay chain
209
Pb( 58 Fe,n) 265 108(<J -0.02 nb) 10-36-MeV a. -1.8 ms > k n o w n d e C ay chain
209 58 266
Bi( Fe,n) 109(<T -0.015 nb) H.l-MeV «• -3.5 ms > i c n o w n d e c a y c h a in

The name Nielsbohrium (Ns) was proposed by the GSI group in recognition of the
suggestion of use of the "cold fusion" reaction and experiments done on element 107
by the Russian group at Dubna who had earlier suggested this name for element 105.
The name Hassium (Hs) was suggested in honor of the state of Hesse where the
experiments had been performed, and Meitnerium (Mt) was proposed in honor of the
famous woman scientist Lise Meitner who was instrumental in the discovery of nuclear
fission and in explaining and interpreting this new phenomenon.
These names were also approved by the ACS in 1994 for use in their journals.

4.3. ELEMENTS 110 THROUGH 112

As the cross sections for the production of still heavier elements and the expected half-
lives dropped, it became necessary to improve the efficiency and discrimination of
existing on-line separator systems. Thus, considerable time elapsed between the
discovery of element 109 and the reports of the discovery of element 110.

4.3.1. Element 110


The first report of possible evidence for the production of element 110 at the
SUPERHILAC at Berkeley in 1991 was made by A. Ghiorso et al. in 1994 and 1995
[50], based on the partial decay chain of one event The newly improved gas-filled
Small Angle Separator SYstem (SASSY-2) was used to separate and identify products
from the following reaction:

209
Bi( 5 9 Co,n) 2 6 7 110 (a -1 pb) "-6-MeVa, ~ 4 m s > ( 1 event)

S. Hofmann et al. [51], using the SHIP whose efficiency and detection system had been
greatly improved, performed experiments during November and December of 1994 at
the UNDLAC, GSI, Germany and in 1995 reported identifying two new isotopes of
element 110 in the following reactions:
208
Pb( 6 2 Ni,n) 2 6 9 110(c~4 pb) n-l-MeVcc,0.17ms > ( 3 events)

208pb(64Nin)271 j 10((J_15 pb) 10.7-MeVoc, 1.1ms >(9events)

A combined Dubna-Lawrence Livermore National Laboratory (LLNL) team led by Yu.


A. Lazarev performed experiments at the Dubna Cyclotron using the Dubna gas-filled
recoil separator during September to December, 1994 and in 1995 reported [52]
evidence for one event of element 110 produced in the following "hot fusion" reaction:

244
Pu( 3 4 S,5n) 2 7 3 l 10(CJ~0.4 p b)"-*-MeV a. 0.3 ms > ( 1 event)

Different isotopes of element 110 were produced in all of these reactions, so none can
be considered confirmation of the others; however, the half-lives and cross sections all
appear to be reasonable. Clearly, the group of S. Hofmann has more convincing data
for their discoveries of ^ ° " l l 0 and ^'M10. No name has as yet been proposed for
element 110.

4.3.2. Element HI
The same group of S. Hofmann et al. also reported [53] identification of three atoms
of element 111 using the SHIP at GSI with rather complete supporting decay chains
formed in the following reaction:
209
Bi( 6 4 Ni,n) 2 7 2 l 1 l(a-3.5 pb) 10-8-MeVa. 1.5 ms > ( 3 events)

No name has yet been proposed for this element.

10
4.3.3. Element 112
Additional experiments carried out by S. Hofmann et al. in February, 1996 [54] at GSI
using SHIP resulted in the identification of two decay chains of element 112
produced in the following reaction:
208
Pb( 7 0 Zn,n) 2 7 7 l 12(c-3.5 pb) 11.45,11.65-MeVq,~0.3 ms >(2 events)

Again, no name has yet been proposed for this element

4.4. HEAVY ELEMENT NAMING

In 1987, the IUPAP and the IUPAC appointed a new Transfermium Working
Group (TWG) to assign credit for discovery of the elements heavier than fermium
(element 100) even though names for the elements through 103 had been approved
previously by IUPAC. Their report assigning credit for discovery of elements 101
through 109 was published in 1993 [55] and proved to be rather controversial in the
cases of elements 102,104, and 105. Subsequent to this, the IUPAC Commission on
Nomenclature of Inorganic Chemistry (CNIC), A. M. Sargeson, Chair, presented [56]
a rather different list of names for elements 103 through 109 to the IUPAC Council
than had been proposed by the acknowledged discoverers; notable were the proposed
names for elements 106 through 108 about which there was no controversy.
Rutherfordium (Rf) was assigned to element 106 and seaborgium for element 106 was
thrown out because of an ex post facto ruling that an element could not be named after
a living person and Glenn T. Seaborg is still alive. Bohrium (Bh) was proposed for
element 107 instead of Nielsbohrium (Ns); hahnium was moved from element 105 to
element 108, replacing the discoverers proposed name of Hassium (Hs) for element
108. Only Lawrencium (Lr) for element 103 (previously approved by IUPAC) and
Meitnerium (Mt) for element 109 were accepted! Dubnium (Db) for element 104 and
Joliotium (Jl) for element 105 replaced Rutherfordium (104) and Hahnium (105)
which have been in common usage for these elements for some 25 years. This change,
together with shifting Rutherfordium to element 106 and Hahnium to element 108,
has created a chaotic situation in heavy element nomenclature, especially since many
studies on the chemical properties of these elements have been published using the
other names. Because of the controversy surrounding these new IUPAC names,
IUPAC decided to return them to "provisional" status and the CNIC invited
comments on them until May 31,1996 and they are currently being reconsidered.

5. Future

The production of elements 2 6 7 , 2 6 9 U Q and ^ ^ 1 1 1 in "cold fusion" reactions with


cross sections of a few pb and of 2 ^ 1 1 0 with a cross section of -15 pb, the estimate
of-0.4 pb for the "hot fusion" rextion to produce ^^\\0, and the cross section o f - 1
pb for the cold fusion reaction to produce ^^^112 make it appear feasible to produce
and detect elements 113 and 114 as well. Somewhat lower cross sections are estimated

11
for the cold fusion reactions of ^Ozn o r . ^ G e with Pb or Bi to produce elements 113
and 114, but these should be within the reach of the SHIP group. A more efficient
gas-filled separator with an opening angle of 12.2° for compound-nucleus recoils
compared to 3.6° for SHIP has been proposed by K. Gregorich et al. [57] at Lawrence
Berkeley National Laboratory; this Berkeley Gas-filled Separator (BGS) should
provide access to nuclides with still lower production cross sections, and would be
particularly advantageous for asymmetric reactions which have a broad angular
distribution, including that resulting from scattering of recoils in the target itself.
Thus thicker targets can be used and it appears promising to use the BGS with its
higher sensitivity to reinvestigate the following more asymmetric "hot fusion"
reactions:

244p u ( 48 C a ,4n)288ll4

248
C m ( 4 8 C a , 4 n ) 2 9 2 l 16 (earlier limit of 200 pb set for half-lives >lms)

With the expected efficiency of the BGS, a cross section of 1 pb should result in the
detection of nearly two events per week. Thus it now appears possible to reach the
long sought superheavy elements in the region of the spherical Z=l 14 shell, but with
fewer neutrons than the N=184 spherical shell.

Acknowledgements

The author wishes to thank her colleague and friend Diana M. Lee for her invaluable
help in producing the figures and her support during preparation of this paper.

Work performed under the auspices of the U.S. Department of Energy by the
Lawrence Livermore National Laboratory under Contract W-7405-Eng-48.

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32. Flerov, G. N., Oganessian, Yu. Ts., Lobanov, Yu. V., Kuznetsov, V. I., Drain, V. A., Perelygin, V. P.,
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13
the Isotope of Element 104 with Mass Number 260, Atomnaya Energ. 17,310; Phys. Lett. 13,73.
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14
55. Wilkinson, D. H., Wapstra, A. H., Ulehla, I., Barber, R. C , Greenwood, N. N., Hrynkiewicz, A.,
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2419-2421.
57. Gregorich, K., private communication, 1996.

15
1 2
He
n
3 4 5 6 7 8 9 10
Li Be B C N o F Ne
11 12 13 14 15 16 17 18
Na MB Al Si P S Cl Ar
19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36
IC Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Sc Br Kr
37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54
Rb Sr Y Zr Nl) Mo Tc Ru Rh Pd Ag Cd Tn Sn Sb Te I Xe
55 56 57 72 73 74 75 76 77 78 79 80 81 82 83 84 85 86
Cs Ra La Ilf Tn \V Re Os Ir Vt An "g TI PI) Bi Po At Rn
87 88 89 104 105 106 107 108 109 110 111 112
(113) (114) (115) (116) (117) (M8)
Fr Ra Ac Rf Ila Sg Ns iis Mt
t
58 59 60 61 62 63 64 65 66 67 68 69 70 71
Lnnthanidcs Ce Pr Nd Pm Sm En Gd Tb Dy Ho Er Tm Yb Lu
90 91 92 93 94 95 96 97 98 99 100 101 102 103
Actinidcs Th Pa U Np Pu Am Cm Bk Cf Es Fm Md No Lr

Figure I. Periodic table as of mid-1996.


1 2

H He

4 5 6 7 8 •i 10
Li Be B C N O F Ne
11 12 U 14 15 16 17 18
Na Mg AI Si P S Gl Ar
iy 20 21 22 Zi 24 25 26 27 2a 2!) JU jl 32 Ji J4 J5 ib
K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr
il J8 jy 40 41 42 <4i) 44 45 46 47 48 4y 51 52 SJ 54
su
Rb Sr Y Zr Nb Mo Ru Rh Pd Ag Cd In Sn Sb Te I Xe
55 56 57-71 12 li 74 75 76 77 78 79 80 81 82 a 84 86
Cs Ba U-Lu Hf Ta W Re Os Ir Pt Au Hg TI Pb Bi Po Rn
(til) an sy yu HI y2 (it4j (9i) (i»6) 100)
Ra Ac Th Pa u
3/ 3a 6U (6i; 62 6J 64 63 66 6; 63 6y /u n
La Ce Pr Nd Sm Eu Gd Tb Dy Ho Er Tm Yb Lu

Figure 2. Periodic table before world war II

1 2
H He

•> 4 2 6 / a y lu
Li Be B c N O F Ne
11 12 1J 14 15 lo 17 18
Na Mg AI Si P S CI Ar
iy 21) 21 22 2J 24 25 26 27 23 2y JU Jl J2 JJ J4 J5 Jo
K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr
J7 Ja jy 4U 41 42 4J 44 45 46 47 48 4y 21) 51 52 5j 54
Rb Sr Y Zr Nb Mo Ru Rh Pd Ag Cd In Sn Sb Te 1 Xe
23 20 57 72 /j 74 75 7o 77 78 79 80 81 52 8j 8-t 85 8b
Cs Ba LJ Hf Ta W Re Os Ir Pt Au Hg T1 Pb Bi Po Rn
87 as yi y3 yo
Ra Ac

Th Pa u Np Pu

Si sy 00 61 02 Oj 04 02 00 67 oy /U 71
Lanthanides
La Ce Pr Nd Sm Eu Gd Tb Dy Ho Er Tm Vb Lu
sy yu yi y~ yj 94 ys yo
AcTinidcs Ac Th Pa V Np Pu

Figure 3. Representation of Seaborg's 1945 periodic table showing an actinide series.


I -u I 1
10,22 U - \
\
O
.O D
\ *
\ O^ .o\

-A

5 to 1 19
V. A
\
\ \
0
A 0-0
\
V ' O
E 1018 —
o
U
\ v O
A 1—1

117 o Hutch \ LJ
Si
40 moles neutrons/cm2 Av * \
E
20-200'kl
10 16
A Cyclamen V^•A b--° U

IS moles neutrons/cm
13 kt \

1O' S
L_
a Mike
10.0OO kt \ _

10' —
! I 1
240 245 250 255 260
number

Figure 4. Production yields for different tests.


101 Md -

238 240 242 244 246 248 250 252 254 256 258

Mass Number (A)


Figure 5. Production of uranium isotopes in the "Mike" thermonuclear
device, and their subsequent decay to beta-stable nuclei.
277
112 240 us
«
272
111 1.5ms
a

267 ? 269 271 27 3?


110 4 us 0.17ms 1.4ms .1s 1ms
a a
a a
266 268
109 Mt 3.4ms 70ms
a a
263 264 265 267 269
108 Hs ? 0.5ms 2ms 20-70
msa 9s
a a, SF? « a | a
261 262 264
107 Ns 12ms 0.44s
6ms 10.1
a, SF? a \a a
258 259 260 261 263 265 266
106 sg 2.9ms 4ms
[Link] 0.3s 0.9s 2-30 » 20-30 >
a a,SF [Link] [Link]? SF.a a a
255 257 25B 260 261 262 263
105 Ha 1.5s 1.33 4.4s 1.5S 1.8s 34s 278
SF a,SF EC,« [Link] a,SF Ec.a SF.a
253 254 ? 255 2S6 257 258 259 260 261 262 263 7
104 Rf 1.4s 7ms [Link] 13ms 3.0s 65s 2a
1.5 s 0.5ms 20ms m
SF SF.O7 a,SF a,SF SF.a? [Link] SF a,SF? SF SF
IF
253 251 255 256 257 258 259 260 261
252
103 Lr 1.3 S 13 3 22 a 26 s 0.65 S 3.9 s 6.1 s 3m 39 m
7 a a a,ec a , EC O,EC a [Link] [Link] SF
150 152 154 156 158 160 162 164 N
Figure 6. Known (rnns-nnhclium isotopes, mid-1906.
Technical Information Department • Lawrence Livermore National Laboratory
University of California • Livermore, California 94551

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