Natural fission chain-reactors on Earth
Criticality in nature is uncommon. At three ore deposits at Oklo in Gabon, sixteen sites (the so-called Oklo Fossil Reactors) have been discovered at which self-sustaining nuclear fission took place approximately 2 billion years ago. Unknown until 1972 (but postulated by Paul Kuroda in 1956[3]), when French physicist Francis Perrin discovered the Oklo Fossil Reactors, it was realized that nature had beaten humans to the punch. Large-scale natural uranium fission chain reactions, moderated by normal water, had occurred far in the past and would not be possible now. This ancient process was able to use normal water as a moderator only because 2 billion years before the present, natural uranium was richer in the shorter-lived fissile isotope 235U (about 3%), than natural uranium available today (which is only 0.7%, and must be enriched to 3% to be usable in light-water reactors).
Artificial nuclear fission
New Zealander, Ernest Rutherford is credited with splitting the atom in 1917.[4] His team in Manchester, England bombarded nitrogen with naturally occurring alpha particles from radioactive material and observed a proton emitted with energy higher than the alpha particle. In 1932 his students John Cockcroft and Ernest Walton, working under Rutherford's direction, attempted to split the nucleus by entirely artificial means, using a particle accelerator to bombard lithium with protons, thereby producing two helium nuclei.[5]
After English physicist James Chadwick discovered the neutron in 1932,[6] Enrico Fermi and his colleagues in Rome studied the results of bombarding uranium with neutrons in 1934.[7] The first person who mentioned the idea of nuclear fission in 1934 was Ida Noddack.[8][9]
After the Fermi publication, Lise Meitner, Otto Hahn and Fritz Strassmann began performing similar experiments in Germany. Meitner, an Austrian Jew, lost her citizenship with the Anschluss in 1938. She fled and wound up in Sweden, but continued to collaborate by mail and through meetings with Hahn in Sweden. By coincidence her nephew Otto Robert Frisch, also a refugee, was also in Sweden when Meitner received a letter from Hahn describing his chemical proof that some of the product of the bombardment of uranium with neutrons, was barium and not barium's much heavier chemical sister element radium (barium's atomic weight is about 60% that of uranium). Frisch was skeptical, but Meitner trusted Hahn's ability as a chemist. Marie Curie had been separating barium from radium for many years, and the techniques were well-known. According to Frisch:
Was it a mistake? No, said Lise Meitner; Hahn was too good a chemist for that. But how could barium be formed from uranium? No larger fragments than protons or helium nuclei (alpha particles) had ever been chipped away from nuclei, and to chip off a large number not nearly enough energy was available. Nor was it possible that the uranium nucleus could have been cleaved right across. A nucleus was not like a brittle solid that can be cleaved or broken; George Gamow had suggested early on, and Bohr had given good arguments that a nucleus was much more like a liquid drop. Perhaps a drop could divide itself into two smaller drops in a more gradual manner, by first becoming elongated, then constricted, and finally being torn rather than broken in two? We knew that there were strong forces that would resist such a process, just as the surface tension of an ordinary liquid drop tends to resist its division into two smaller ones. But nuclei differed from ordinary drops in one important way: they were electrically charged, and that was known to counteract the surface tension.
The charge of a uranium nucleus, we found, was indeed large enough to overcome the effect of the surface tension almost completely; so the uranium nucleus might indeed resemble a very wobbly unstable drop, ready to divide itself at the slightest provocation, such as the impact of a single neutron. But there was another problem. After separation, the two drops would be driven apart by their mutual electric repulsion and would acquire high speed and hence a very large energy, about 200 MeV in all; where could that energy come from? ...Lise Meitner... worked out that the two nuclei formed by the division of a uranium nucleus together would be lighter than the original uranium nucleus by about one-fifth the mass of a proton. Now whenever mass disappears energy is created, according to Einstein's formula E=mc2, and one-fifth of a proton mass was just equivalent to 200MeV. So here was the source for that energy; it all fitted![10]
In December 1938, the German chemists Otto Hahn and Fritz Strassmann sent a manuscript to Naturwissenschaften reporting they had detected the element barium after bombarding uranium with neutrons;[11] simultaneously, they communicated these results to Lise Meitner. Meitner, and her nephew Otto Robert Frisch, correctly interpreted these results as being nuclear fission.[12] Frisch confirmed this experimentally on 13 January 1939.[13] In 1944, Hahn received the Nobel Prize for Chemistry for the discovery of nuclear fission. Some historians who have documented the history of the discovery of nuclear fission believe Meitner should have been awarded the Nobel Prize with Hahn.[14][15][16]
Meitner’s and Frisch’s interpretation of the work of Hahn and Strassmann crossed the Atlantic Ocean with Niels Bohr, who was to lecture at Princeton University. Isidor Isaac Rabi and Willis Lamb, two Columbia University physicists working at Princeton, heard the news and carried it back to Columbia. Rabi said he told Enrico Fermi; Fermi gave credit to Lamb. Bohr soon thereafter went from Princeton to Columbia to see Fermi. Not finding Fermi in his office, Bohr went down to the cyclotron area and found Herbert L. Anderson. Bohr grabbed him by the shoulder and said: “Young man, let me explain to you about something new and exciting in physics.”[17] It was clear to a number of scientists at Columbia that they should try to detect the energy released in the nuclear fission of uranium from neutron bombardment. On 25 January 1939, a Columbia University team conducted the first nuclear fission experiment in the United States,[18] which was done in the basement of Pupin Hall; the members of the team were Herbert L. Anderson, Eugene T. Booth, John R. Dunning, Enrico Fermi, G. Norris Glasoe, and Francis G. Slack. The next day, the Fifth Washington Conference on Theoretical Physics began in Washington, D.C. under the joint auspices of the George Washington University and the Carnegie Institution of Washington. There, the news on nuclear fission was spread even further, which fostered many more experimental demonstrations.[19]
Frédéric Joliot-Curie's team in Paris discovered that secondary neutrons are released during uranium fission, thus making a nuclear chain-reaction feasible. The figure of about two neutrons being emitted with nuclear fission of uranium was verified independently by Leo Szilárd and Walter Henry Zinn. The number of neutrons emitted with nuclear fission of 235U was then reported at 3.5/fission, and later corrected to 2.6/fission by Frédéric Joliot-Curie, Hans von Halban and Lew Kowarski.
The fission chain reaction
"Chain reactions" at that time were a known phenomenon in chemistry, but the analogous process in nuclear physics, using neutrons, had been foreseen as early as 1933 by Szilárd, although Szilárd at that time had no idea with what materials the process might be initiated (Szilárd thought it might be done with light neutron-rich elements). Szilárd, a Hungarian born Jew, also fled mainland Europe after Hitler's rise, eventually landing in the US.
With the news of fission neutrons from uranium fission, Szilárd immediately understood the possibility of a nuclear chain reaction using uranium. In the summer, Fermi and Szilard proposed the idea of a nuclear reactor (pile) to mediate this process. The pile would use natural uranium as fuel, and graphite as the moderator of neutron energy (it had previously been shown by Fermi that neutrons were far more effectively captured by atoms if they were moving slowly, a process called moderation when the neutrons were slowed after being released from a fission event in a nuclear reactor).
In August Hungarian-Jewish refugees Szilard, Teller and Wigner thought that the Germans might make use of the fission chain reaction. They decided to warn President Roosevelt of this possible German menace, and persuaded German-Jewish refugee Albert Einstein to lend his name. The Einstein–Szilárd letter suggested the possibility of a uranium bomb deliverable by ship, which would destroy "an entire harbor and much of the surrounding countryside." The President received the letter on 11 October 1939 — shortly after World War II began in Europe, but two years before U.S. entry into it.
In England, James Chadwick proposed an atomic bomb utilizing natural uranium, based on a paper by Rudolf Peierls with the mass needed for critical state being 30–40 tons. In America, J. Robert Oppenheimer thought that a cube of uranium deuteride 10 cm on a side (about 11 kg of uranium) might "blow itself to hell." In this design it was still thought that a moderator would need to be used for nuclear bomb fission (this turned out not to be the case if the fissile isotope was separated).
In December, Heisenberg delivered a report to the German Ministry of War on the possibility of a uranium bomb.
In Birmingham, England, Frisch teamed up with Rudolf Peierls, another German-Jewish refugee. They had the idea of using a purified mass of the uranium isotope (235U). They determined that an enriched 235U bomb could have a critical mass of only 600 grams, instead of tons, and that the resulting explosion would be tremendous. (The amount actually turned out to be 15 kg, although several times this amount was used in the actual uranium (Little Boy) bomb). In February 1940 they delivered the Frisch–Peierls memorandum. Ironically, they were still officially considered "enemy aliens" at the time.
Glenn Seaborg, Joe Kennedy, Art Wahl and Italian-Jewish refugee Emilio Segrè shortly discovered 239Pu in the decay products of 239U produced by bombarding 238U with neutrons, and determined it to be fissionable like 235U.
On June 28, 1941, the Office of Scientific Research and Development was formed in the U.S. to mobilize scientific resources and apply the results of research to national defense. In September, Fermi assembled his first nuclear "pile" or reactor, in an attempt to create a slow neutron induced chain reaction in uranium, but the experiment failed for lack of proper materials, or not enough of the materials which were available.
Producing a fission chain reaction in natural uranium fuel was found to be far from trivial. Early nuclear reactors did not use isotopically enriched uranium, and in consequence they were required to use large quantities of highly purified graphite as neutron moderation materials. Use of ordinary water (as opposed to heavy water) in nuclear reactors requires enriched fuel — the partial separation and relative enrichment of the rare 235U isotope from the far more common 238U isotope. Typically, reactors also require inclusion of extremely chemically pure neutron moderator materials such as deuterium (in heavy water), helium, beryllium, or carbon, the latter usually as graphite. (The high purity for carbon is required because many chemical impurities such as the boron-10 component of natural boron, are very strong neutron absorbers and thus poison the chain reaction.)
Production of such materials at industrial scale had to be solved for nuclear power generation and weapons production to be accomplished. Up to 1940, the total amount of uranium metal produced in the USA was not more than a few grams, and even this was of doubtful purity; of metallic beryllium not more than a few kilograms; concentrated deuterium oxide (heavy water) not more than a few kilograms. Finally, carbon had never been produced in quantity with anything like the purity required of a moderator.
The problem of producing large amounts of high purity uranium was solved by Frank Spedding using the thermite process. Ames Laboratory was established in 1942 to produce the large amounts of natural (unenriched) uranium metal that would be necessary for the research to come. The critical nuclear chain-reaction success of the Chicago Pile-1 (December 2, 1942) which used unenriched (natural) uranium, like all of the atomic "piles" which produced the plutonium for the atomic bomb, was also due specifically to Szilard's realization that very pure graphite could be used for the moderator of even natural uranium "piles". In wartime Germany, failure to appreciate the qualities of very pure graphite led to reactor designs dependent on heavy water, which in turn was denied the Germans by Allied attacks in Norway, where heavy water was produced. These difficulties prevented the Nazis from building a nuclear reactor capable of criticality during the war.
For more detail on the early development of the first nuclear reactors and nuclear weapons, see Manhattan Project.
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