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WILLIAM DRAPER HARKINS December 28, 1873-March 7, 1951 BY ROBERT S. MULLIKEN WILLIAM DRAPER HARKINS was a remarkable man. Although he was rather late in beginning his career as professor of physical chemistry, his success was outstanding. He was a leader in nuclear physics at a time when American physicists were paying no attention to nuclei. Besides this, his work in chem- istry covers a broad range of physical chemistry, with especial emphasis on surface phenomena. He was a meticulous and re- sourceful experimenter, as well as an enterprising one, who did not hesitate to enter new fields and use new techniques. He participated broadly, not only in the development of pure science but also in its industrial applications. Harkins was born December 28, 1873, the son of Nelson Goodrich Harkins and Sarah Eliza (Draper) Harkins, in Titus- ville, Pennsylvania, then the heart of the new, booming oil industry. At the age of seven, he invested his entire capital of $12 in an oil well that his father had drilled in the Bradford, Pennsylvania, fields. This investment returned his capital several times. Fortunately for science, the returns were not great enough to attract him permanently into oil production. In 1892, at the age of nineteen, Harkins went to Escondido, California, near San Diego, to study Greek at the Escondido Seminary, a branch of the University of Southern California. The courses of study are described in the University of Southern 49

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so BIOGRAPHICAL MEMOIRS California Year-Book for 1891-1892, where Harkins is listed as a student. Apparently, the seminary (now the Escondido High School) served as a preparatory school for the university. Harkins attended the seminary for one year, but had to learn Greek elsewhere because it was discontinued the year he came; he enrolled in a general arts course. It seems that Harkins spent a few more years in Escondido, and made many friends, but there is no other information as to his activities while there. Harkins entered Stanford University in 1896 at age twenty- three and received an A.B. in chemistry in 1900, at twenty-six. In 1898-1900, he was assistant, then instructor, in chemistry at Stanford. For the next twelve years, Harkins was professor and head of the Department of Chemistry of the University of Montana at Missoula, but he spent a considerable amount of time in postgraduate and postdoctoral work elsewhere. He did postgraduate work at the University of Chicago in 1901 and 1904, and at Stanford University, 1905-1906, culminating in a Ph.D. in chemistry from Stanford on June 10, 1908. He did re- search in Germany in 1909 and was at the Massachusetts In- stitute of Technology as research associate in 1909-1910. Harkins left Missoula in 1912 at age thirty-nine for an appoint- ment at the University of Chicago, where he conducted further research the remaining thirty-nine years of his life. In Missoula, Harkins took part in the life of the city and state: He was President of the Missoula City Board of Health from 1906 to 1912. He was chemist in charge of smelter in- vestigations for the Anaconda Farmers Association (1902-1910), the Montana Copper Company of California (1904), and the U.S. Department of Justice (1910-1912~. His first four scientific papers, published during the period 1907-1910, are devoted to arsenical poisoning of animals by smelter smoke, and related matters. In 1911 Harkins did some research for the Carnegie Institution of Washington. On June 9, 1904, he married Anna Louis Hathaway, who was head of the Department of English

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WILLIAM DRAPER HARKINS ~1 at the University of Montana. She had also been a graduate student at the University of Chicago. At the University of Chicago, with the opportunity to con- duct pure research and to work with graduate students, Harkins' advancement was rapid. He was first assistant professor of general chemistry ~ 1912-1914), then associate professor ~ 1914- 1917), then professor of physical chemistry. In 1916-1917 he was a professorial lecturer at the Mellon Institute for Industrial Research, and he lectured at the University of Illinois (1918- 1919~. In 1935 he was appointed Andrew MacLeish Distin- guished Service Professor at Chicago. He was George Fisher Baker Lecturer at Cornell University in 1936-1937. In 1939 he retired officially at Chicago, but continued research with undiminished vigor until his death in 1951. During World War I, early in 1915, Harkins began work on explosives for the Allies. Later in the war, he did special work for the army and the Chemical Warfare Service. Throughout his career, while carrying on notable work In pure science, he also contributed to applied science: as a consulting chemist with the U.S.13ureau of Mines, 1920-1922; consulting engineer, U.S. Air Service, 1924-1927; and consulting chemist, Chemical Warfare Service from 1927, Libby-Owens-Ford Glass Company from 1929, Universal Oil Products Company, 1930-1951, and United States Rubber Company, 1939-1941. During World War II, he was a member of the National Defense Research Committee (1941-1945~. Civically, he also participated as a member of the Chicago Commission on Ventilation (1916- 1928~. Harkins was also active in the affairs of the American Chem- ical Society. He was editor of the section of General and Physical Chemistry of Chemical Abstracts (1939-1951), chairman of the Chicago Section (1915-1916), chairman of the Division of Phys- ical and Inorganic Chemistry ~ 1919-1920), and councillor-at- large for a time. He was the recipient of the Willard Gibbs

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52 BIOGRAPHICAL MEMOIRS Gold Medal of the American Chemical Society on May 28, 1928, in recognition of his work in surface chemistry and on nuclear structure and isotopes. He was also a vice president (chemistry) of the American Association for the Advancement of Science. Harkins was elected a member of the National Academy of Sciences in 1921, and at the annual meetings in Washington in April he took a lively part in the discussions. He was also a member of the American Philosophical Society, to which he was elected in 1925. In Chicago, Harkins always lived with his family near the university (at 5437 Ellis Avenue). He and his wife had two children, Henry Nelson Harkins and Alice Marion Harkins. Henry Harkins (born in Missoula in 1905) obtained B.S. and M.S. degrees in physical chemistry, a Ph.D. in medicine (1928), and an M.D. in 1931, all at Chicago. He went on to a distin- guished career in surgery. His M.S. thesis on surface tension of blood serum was completed under his father's direction in 1926. Marion Harkins won success as a concert singer. The members of the family were devout Episcopalians. The Harkins family had a summer home on Lake Michigan, at Lakeside, across the lake from Chicago. An active mountain climber in his youth in California and Montana, Harkins visited the Rockies annually for many years. At the time of his death, he had been paying daily visits to the hospital after Mrs. Harkins had suffered a stroke. Harkins' contributions to pure science covered a wide spec- trum in the field of physical chemistry, extending also into physics. When I came to Chicago as a graduate student in 1918, it was because I had read about Harkins' pioneering work toward the understanding of nuclear structure, a subject ignored at that time by American physicists. In fact, during the period 1913-1928, Harkins and his students were the only ~ G. EgIoff, "Fathers and Sons 22(1944):804. in Chemistry," Chemical and Engineering News

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WILLIAM DRAPER HARKINS 53 Americans engaged in work relating to the structure of the atomic nucleus. A perusal of the bibliography of Harkins' papers gives a perspective of his scientific interests and of his graduate students and other collaborators. In 1915 the diversity of his interests is already evident. His most extensive work was in surface chemistry (1 15 papers) and in nuclear and atomic structure and isotope separation (nearly 80 papers). On the occasion when he received the Willard Gibbs medal, Harkins gave an address that shows something of his personality and the beginnings of his activity in his major fields of research. Following is a quotation from the introductory part of his talk. 1 _ r_ ~ _ _ _ . , ~ . . _ "As an undergraduate, research appealed to me as one of arc ~ ~,~:~r cures, ana 1 was attracted both to the very large, in astronomy, and to the extremely minute, in chemistry and physics. While the study of the atom and of radioactivity, then a new subject, had an extreme fascination, there were two subjects of investigation in physical chemistry which seemed to me of such minor importance that I took a firm resolution never to be enticed into working on either of them. "These two fields of work were surface tension and solu- bility. To illustrate, let us consider surface tension. I did not realize that the importance of the study of surfaces and surface energy arises from the fact that the surface lies outside every body, particle or cell. To get inside from outside or outside from inside, the surface must be traversed. "In 1909 I went to Germany to study with Fritz Haber, the chemist whose work on the synthesis of ammonia lengthened the World War by one or two years. On the first day of my stay in Karlsruhe, he invited me to lunch with him and his assistant at the leading, hotel of the city. "Haber insisted that as a visiting professorI was then pro- fessor of chemistry at the University of Montanaonly a prob-

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~4 BIOGRAPHICAL MEMOIRS lem of extreme importance should be given to me. He and his assistant rose, drank my health, and Haber said, 'He shall work on surface tension.' Unfortunately, or fortunately, I knew hardly enough German to object, and when much later I found that many of the world's greatest scientists had been interested in surface phenomena, I was thankful for this lack of knowl- edge." The work revealed to Harkins the fascinating problems of surface chemistry and initiated his highly original work in that field. When he was able after his establishment in Chicago to resume that work, he began his investigation of the orientation of molecules in surfaces. He was one of the three (the others were W. G. Hardy and Irving Lan~muir) who independently suggested the theory of orientation of molecules in surfaces. At Chicago in the winter quarter of 1913-1914, Harkins gave the earliest series of lectures on the theory of this subject. Thus began a long chain of steps, from improved experiments to improved theory to new experiments, which characterized Harkins' work in surface chemistry and related fields for forty years. The sequence was particularly fruitful because Harkins combined meticulous and ingenious experimental techniques with a knack for original interpretation of data. Now continu- ing the quotation from Harkins, '`After the completion of the experimental work, I returned to America in order to work on physical chemistry with A. A. Noyes and G. N. Lewis, both of whom have been awarded the Gibbs Medal. Here I met my second aversion, for A. A. Noyes stated that, under the grant from the Carnegie Institution which supported the work, it was expected that the general subject of research should be the theory of solutions, but the special subject solubility." In the last year of his life, Harkins completed a book, pub- lished in 1952, Physical Chemistry of Surface Films, summariz- ing his work on the subject. The book contains an introduction

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WILLIAM DRAPER HARKINS 55 by Thomas F. Young, a younger colleague and a great admirer of Harkins. This introduction contains a paragraph that com- ments interestingly on the fruits of Harkins' work at M.I.T.: "During the brief period which Dr. Harkins spent at the Massachusetts Institute of Technology in 1909-10, Professor A. A. Noyes was greatly interested in theories of solutions, and inspired an outstanding group of young men to investigate the subject. A remarkable series of papers came from the lab- oratory describing work done by or under the direction of A. A. Noyes, G. N. Lewis, W. C. Bray, W. D. Harkins, and others. Of course Harkins did not know then how important that work on the thermodynamics of electrolytic solutions would be to his own later investigations of surface phenomena, especially his studies of adsorption. In 1911 he published three papers presenting his researches on solubility carried out at the Massachusetts Institute of Technology. In later years he contributed about ten more papers on ionic interactions. The work of A. A. Noyes and his group aided G. N. Lewis in his discovery of the ionic strength principle. The latter once re- marked that the principle was obtained within a few hours after he had picked up notes of a conference held some ten years earlier with Harkins." Continuing further with the quotation from Harkins' Gibbs Medal address, first about his work on surface chemistry, "Now the greatest of solubility rules is 'similia similibus solv- This rule suggested that the experiments on surface tension might have given results more in accord with the theory if more complicated molecules, such as those present in the muscles, had been used. It is advisable, however, in scientific work, to use as simple materials as will give the desired behavior, so substances like butyric acid were con- sidered.... a molecule of this substance possesses the interesting characteristic that at one end it is like oil, and at the other like water. untur' or 'like dissolves like.'

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56 BIOGRAPHICAL MEMOIRS "Thus we may place a thick layer of oil on water and add butyric acid. The water-like ends of the molecules should be soluble in water, and the oil-like ends in the oil, but only at the interface between the two can both ends of the molecule be satisfied at the same time. From this point of view the butyric acid should be very much more soluble at the interface than in either oil or water, which is true. Furthermore, at the interface there should be a certain structure, since the molecules of butyric acid should, in general, be oriented with oil-like ends toward the oil, and water-like ends toward the water.... "A later careful search in the literature showed that Hardy, a noted English biologist, had just suggested (1912) that since a surface is extremely unsymmetrical with reference to the material on its two sides, the molecules in the surface should be oriented. Thus the theory of dissymmetry and that of solu- hility gave rise in two different minds to the same suggestion." Especially in his later papers, Harkins deals extensively with emulsion polymerization, soap micelles, and other matters related to the formation of colloids. He also deals with adsorp- tion and with the surfaces of solids and their interaction with liquids. Again, in the Gibbs Medal address, Harkins explains his interest in atomic nuclei as follows: "In order to understand the action of surfaces, it appeared essential to learn as much as possible about the electrical struc- ture of molecules and of atoms, so, in 1913, I began to study more intensively the current theories of atomic structure. In 1904, Nagaoka had suggested that an atom consists of a central sun or nucleus and a system of negative electrons as satellites. This theory was amplified by Rutherford, who showed that the positively charged atom nucleus appears to be extremely minute in comparison with the space occupied by the atom. For many years the phenomena of radioactivity had been extremely fasci- nating to me, and this was undoubtedly what caused my atten- tion to be directed more specially to the nucleus, which de-

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WILLIAM DRAPER HARKINS 57 "ermines the stability and even the existence of the atom as a whole." A series of three papers by Harkins and his student E. D. Wilson in 1915 represents the first of a number of papers pub- lished over the years in which Harkins developed ideas on the structure of atomic nuclei. The papers distinguish carefully between chemical elements and atomic species. In general, an element is a mixture of atomic species (isotopes). In 1915 it was already clear that most of the lighter elements have atomic weights very close to a unit that is slightly (about 0.77 percent) less than the mass of the hydrogen atom. The 0.77 percent dis- crepancy was attributed by Harkins and Wilson (and also inde- pendently by Rutherford and others) to what they called a "packing effect," ascribed to a loss of mass predictable from Lorentz' electromagnetic theory if protons and electrons inter- act at sufficiently close range. They included a speculation that the conversion of hydrogen to helium might be a source of the energy for the sun and stars. Harkins' friend A. C. Lunn, pro- fessor of mathematical physics, made the calculations for him. As time went on, it became increasingly clear from mass spec- troscopic evidence that those elements whose atomic weights differ from integral multiples of the basic unit are mixtures . of Isotopes. Quoting G. N. Lewis Whys. Rev. 46~1934~:897], "It was Harkins who first called attention to the striking connection between the atomic weights of the elements and their abun- dance, not only in the earth's crust, but fas a much better sample of the solar system], in the meteors." And it was he who first used these abundances as criteria for the relative stabilities of various atomic species. After E. Rutherford's proof of the nuclear atom, and until the experimental proof by J. Chadwick in 1932 of the independent existence of the neutron, it was generally believed that nuclei are built of protons (not so named at first) and electrons. Harkins noticed that the relative abun-

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58 BIOGRAPHICAL MEMOIRS dances, hence stabilities, of different atomic species are by far greater for nuclei containing an even number of protons and electrons; the next class, in terms of abundance, contains an odd number of protons and an even number of electrons. Two much rarer classes contain an even number of protons but an odd number of electrons, or odd numbers of both protons and electrons. It was also apparent to Harkins that many of the lighter species (e.g., ]2C, 160, 20Ne) could be thought of as built of ~-particles; the -particle itself, the helium nucleus, being a very stable composite, formed by close packing of four protons and J ~ ~ A A ~ _ ~ two electrons, pees. The atomic weights of the a! composites such as ~2C and t60 showed little further packing effect. Harkins did not attempt to give a categorical answer to the question of whether such nuclei consist of (nearly unchanged) ~-particles, or whether they merely could be built from ~-particles. It was of course known that -particles can have an independent existence. In a similar way, Harkins concluded that nuclei such as those of OF and 23Na could be built from, or possibly consist of, -particles plus a hvt)otheticn1 1,-n~rtirle {noun M~rlrinc rare tioned, but did not emphasize, the possibility of the inde- pendent existence of this and other particles (the helion, p4e4; p2e; the ~ particle, pees; and a particle pe). He mentioned that pees and p2e, since known, would be isotopes of hydrogen (the triton, and the deuteron). Rutherford entertained similar ideas, and independently (and earlier than Harkins) spoke of packing (of H to form He), but it was Harkins who made the major contributions on the stabilities of atomic species and the structure of nuclei. This work culminated in his "new periodic system" of atomic species expressed in a diagram of "isotonic ~ ~ ~ A_ 1~ ~ ~ = ~ ~ T ~ ~ 1 - -A ~ ~ rat \r~-~/~ ,, $~1A- V - _ _ c~-susaromlc number. Here, if the structure of any nucleus is written as (p2e)Z spelt, n is the isotopic number if Z is the atomic number; n was later recognized as a neutron number.

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WILLIAM DRAPER HARKINS 71 With H. E. Bowers. The carbon-halogen bond as related to Raman spectra. i. Am. Chem. Soc., 53:2425. With D. M. Gans. An adsorption method for the determination of the area of a powder. i. Am. Chern. Soc., 53:2804. With D. M. Gans. The direct measurement of the adsorption of soluble substances by the bubble method. I. Phys. Chem., 35:722. 1932 The hydrogen nucleus of mass 2 (isohydrogen nucleus pee) as a unit in atom building. l. Am. Chem. Soc., 54:1256. With R. R. Haun. The Raman spectrum of germanium tetra- chloride. I. Am. Chem. Soc., 54:3917. With R. R. Haun. The vibration of atoms at the end of organic molecules: Raman effect and the carbon-chlorine bond. l. Am. Chem. Soc., 54:3920. With D. M. Gans. Monomolecular films. The solid-liquid inter- face and the sedimentation and flocculation of powders in liquids. I. Phys. Chem., 36:86. With L. W. Ryan and D. M. Gans. Flocculation, dispersion, and settling of pigments in relation to adsorption. Ind. Eng. Chem., 24:1288. With E. K. Fischer. Monomolecular films. The liquid-liquid inter- face and the stability of emulsions. J. Phys. Chem., 36:98. 1933 The neutron, the atomic nucleus and mass defects. l. Am. Chem. Soc., 55:855. The new kind of matter: element zero or neutron. Sci. Mon., 36: 546. With D. M. Gans and H. W. Newson. Atomic disintegration by a relatively slow neutron. Phys. Rev., 43:208. With D. M. Gans and H. W. Newson. A neutron of high velocity, and energy relations for nuclear disintegration by non-capture. Phys. Rev., 43:307. Emission of gamma rays by nuclei excited by neutrons, and nuclear energy levels. Phys. Rev., 43:362. The neutron, atom building and a nuclear exclusion principle. Proc. Natl. Acad. Sci., 19:307. With C. Doede. An apparatus for the separation of isohydrogen (deuterium) oxide by electrolysis. l. Am. Chem. Soc., 55:4330.

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72 BIOGRAPHICAL MEMOIRS With D. M. Gans and H. W. Newson. Disintegration of neon nuclei by fast neutrons. Phys. Rev., 44:236. With D. M. Gans and H. W. Newson. Failure to detect the radio- activity of beryllium with the Wilson cloud chamber. Phys. Rev., 44:310. With D. M. Gans and H. W. Newson. The disintegration of the nuclei of nitrogen and other light atoms by neutrons. I. Phys. Rev., 44:529. With D. M. Gans and H. W. Newson. Disintegration of fluorine nuclei by neutrons and the probable formation of a new isotope of nitrogen (Nisi. Phys. Rev., 44:945. With J. M. Jackson. A spectroscopic study of the decomposition and synthesis of organic compounds by electrical discharges: elec- trodeless and glow discharges. J. Chem. Phys., 1:37. With E. K. Fischer. Contact potentials and the effects of unimolec- ular films on surface potentials. I. Films of acids and alcohols. J. Chem. Phys., 1:852. 1934 Free radicals in electrical discharges. Transactions of the Faraday Society, 30:221. Nomenclature for the isotopes of hydrogen (proto- and deuto-hydro- gen) and their compounds. Science, 79: 138. With D. M. Gans. Atomic disintegration by "non-capture." Nature, 133:794. With D. M. Gans. Inelastic collisions with changes of mass and the problem of nuclear disintegration with capture or non-capture of a neutron, or another nuclear projectile. Phys. Rev., 46:397. With D. M. Gans. Artificial radioactivity and the conversion of kinetic into gamma ray energy associated with nuclear disinte- gration by neutrons. Phys. Rev., 46:827. With D. M. Gans. The emission of gamma rays in nuclear reactions. J. Am. Chem. Soc., 56:2786. With D. M. Gans. The mass of the neutron. Nature, 134:968. With F. E. Kredel and H. N. Harkins. Toxicity of heavy water. Proceedings of the Society for Experimental Biology and Medi- cine, 32:5. 1935 With D. M. Gans and H. W. Newson. The disintegration of the nuclei of light atoms by neutrons. Phys. Rev., 47:52.

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WILLIAM DRAPER HARKINS 73 With H. E. Ries, fir., and E. F. Carman. Surface pressures and po- tentials of long molecules: polymers of omega-hydroxy decanoic acid. J. Am. Chem. Soc., 57:776. With E. F. Carman and H. E. Ries, Jr. Monomolecular Elms of molecules which lie flat on the surface of water. I. Surface pres- sures and potentials of films of long molecules: polymers of omega-hydroxy decanoic acid. I. Chem. Phys., 3:692. With H. E. Ries, Jr., and E. F. Carman. Surface potentials and force-area relations of monomolecular films. II. d-Pimaric and tetrahydro-d-pimaric acids. i. Am. Chem. Soc., 57:2224. 1936 Some relations of carbon and its compounds. Journal of Organic Chemistry, 1 :52. With R. J. Moon. The production of high velocity ions for the disintegration of atomic nuclei. Science, 82:244. Nuclear chemistry, the neutron and artificial radioactivity. Science, 83:533. With M. D. Kamen, H. W. Newson, and D. M. Cans. Neutron- proton interaction: the scattering of neutrons by protons. Phys. Rev., 50:980. With H. E. Ries, in and E. F. Carman. The rearrangement of molecules in monomolecular films: polycyclic compounds of the five ring series. J. Chem. Phys., 4:228. With E. F. Carman and H. E. Ries, fir. The rearrangement of mole- cules in plastic monomolecular films: pressure-area and potential relations for polycyclic compounds of the five ring series. J. Am. Chem. Soc., 58:1377. With R. J. Myers. Polymolecular films. J. Am. Chem. Soc., 58:1817. With R. i. Myers. Hydrogen ion concentration and the behavior and measurement of monomolecular and polymolecular films on water. l. Chem. Phys., 4: 716. With R. l. Moon. An electronic analysis of some surfaces by means of slow electrons. J. Phys. Chem., 40:941. With R. I. Myers. Polymolecular films: mixed films with two or more components. I. Fatty acids and non-polar substances. J. Phys. Chem., 40:959. With R. T. Florence and R. I. Myers. Contact potentials of re- versible soluble films of lauric acid. Nature, 138:405.

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74 BIOGRAPHICAL MEMOIRS 1937 The intermediate nucleus in the disintegrative-synthesis of atomic nuclei: disintegration in steps. Proc. Natl. Acad. Sci., 23:120. The intermediate nucleus and atomic disintegration in steps. Phys. Rev.,51:52. The nuclear exclusion principle and the neutron-proton pattern. Phys. Rev., 52:39. Linear or edge energy and tension as related to the energy of surface formation and of vaporization. J. Chem. Phys., 5: 135. With R. l. Myers. Effects of traces of metallic ions on Elms at inter- faces and on the surface of water. Nature, 139:367. With R. l. Myers. Viscosity of monomolecular films. Nature, 140: 465. ~ . .. . . . With F. M. Fowkes and R. i. Myers. Ultramicroscopic examination of mixed films. l. Am. Chem. Soc., 59:593. With T. F. Anderson. I. A simple accurate film balance of the vertical type for biological and chemical work, and a theoretical and experimental comparison with the horizontal type. II. Tight packing of a monolayer by ions. J. Am. Chem. Soc., 59:2189. With A. R. Brosi. The abundance ratio of the isotopes in natural or isotonically separated carbon. Phys. Rev., 52:472. With R. l. Myers. The viscosity (or fluidity) of liquid or plastic monomolecular films. l. Chem. Phys., 5:601. With E. S. Fetcher, fir., and R. S. Lillie. A method for the investi- gation of electrostenolysis. Journal of General Physiology, 20: 671. With F. A. Long and G. C. Nutting. The surface tension of aqueous soap solutions as a function of hydrogen ion (pH) and salt con- centration. I. Sodium laurate and sodium nonylate. l. Am. Chem. Soc., 59:2197. 1938 With J. G. Kirkwood. The viscosity of monolayers: theory of the surface slit viscosimeter. J. Chem. Phys., 6:53. With R. W. Mattoon. The contact potential of solid films formed by evaporation and by solidification and of built-up multilayers on metals. Phys. Rev., 53:911. With T. F. Anderson. Protein monolayers: films of oxidized cyto- chrome C. l. Biol. Chem., 125: 369.

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WILLIAM DRAPER HARKINS 75 With R. T. Florence. Effect of space isomerism on the squeezing out of an unsaturated compound from a mixed monolayer on an aqueous sub-solution. Nature, 142:913. With R. T. Florence. Molecular interaction in mixed monolayers on aqueous subsolutions. I. Mixtures of alcohols, acids and amines. i. Chem. Phys., 6:847. With F. M. Fowkes. Pressure-area relations of monolayers at the solid-liquid interface. I. Am. Chem. Soc., 60:1511. With L. Fourt. Surface viscosity of long-chain alcohol monolayers. J. Phys. Chem., 42:897. With R. T. Florence. Molecular interaction in mixed monolayers. II. Unstable mixtures with unsaturated acids. i. Chem. Phys., 6:856. 1939 With R. W. Mattoon. Film potentials of stearate multilayers and other dielectrics on metal surfaces. i. Chem. Phys., 7:186. With G. E. Boyd. Viscosity of two-dimensional systems: effect of pressure and temperature, and the detection of phase transitions in monolayers. I. Chem. Phys., 7:203. With G. C. Nutting. Pressure-area relations of fatty acid and alcohol monolayers. i. Am. Chem. Soc., 51: 1180. With E. Boyd. Molecular interaction in monolayers: viscosity of two-dimensional liquids and plastic solids. V. Long chain fatty acids. i. Am. Chem. Soc., 61:1188. With G. C. Nutting. Energy relations in transformations from three to two-dimensional systems. I. The latent heat and entropy of spreading of myristic and pentadecylic acids. l. Am. Chem. Soc., 61:1702. With G. Groetzinger. A new method for the investigation of the electrical properties of multilayers. l. Chem. Phys., 7:204. With W. D. Harkins. Some aspects of surface chemistry funda- mental to biology. Publ. 7, Am. Assoc. Adv. Sci., p. 19. With G. C. Nutting. The pressure-area and pressure-temperature relations of expanded monolayers of myristic and pentadecylic acids. J. Am. Chem. Soc., 61:2040. 1940 With L. Fourt and P. C. Fourt. Immunochemistry of catalase. II. Activity in multilayers. J. Biol. Chem., 132:111.

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76 BIOGRAPHICAL MEMOIRS With T. F. Young and E. Boyd. The thermodynamics of films: energy and entropy of extension and spreading of insoluble monolayers. J. Chem. Phys., 8:954. With L. B. Borst. Search for a neutron-deuteron reaction. Phys. Rev., 57:659. With G. C. Nutting and F. A. Long. The change with time of the surface tension of solutions of sodium cetyl sulfate and sodium lauryl sulfate. l. Am. Chem. Soc., 62:1496. With G. C. Nutting. The viscosity of monolayers: a test of the canal viscosimeter. l. Am. Chem. Soc., 62:3155. With F. M. Fowkes. The state of monolayers adsorbed at the inter- face solid-aqueous solution. l. Am. Chem. Soc., 62:3377. 1941 Surface chemistry. Nature, 148:743. A general thermodynamic theory of the spreading of liquids to form duplex films and of liquids or solids to form monolayers. I. Chem. Phys., 9:552. Surface films of fatty acids, alcohols and esters. Chem. Rev., 29:385. With E. Boyd. The states of monolayers. I. Phys. Chem., 45:20. 1942 Energy relations of the surfaces of solids. I. Surface energy of the diamond. i. Chem. Phys., 10:268. (7' With L. E. Copeland. A superliquid in two dimensions and a first- order change in a condensed monolayer. I. Energy, compressi- bility, and order of phase transformations. i. Chem. Phys., 10: 272. With H. K. Livingston. Energy relations of the surfaces of solids. II. Spreading pressure as related to the work of adhesion be- tween a solid and a liquid. l. Chem. Phys., 10:342. With G. E. Boyd. The energy of immersion of crystalline powders in water and organic liquids. J. Am. Chem. Soc., 64:1190. With G. E. Boyd. The binding energy between a crystalline solid and a liquid: the energy of adhesion and immersion. Energy of immersion of crystalline powders. II. l. Am. Chem. Soc., 64: 1195. With G. E. Boyd. The film balance as an analytical tool for bio- logical and food research. Ind. Eng. Chem., 14:496. With L. E. Copeland and G. E. Boyd. A superliquid in two dimen- sions and a first-order change in a condensed monolayer. II.

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WILLIAM DRAPER HARKINS 77 Abnormal viscosity relations of alcohol monolayers in con- densed liquid phases. J. Chem. Phys., 10:357. With L. E. Copeland. The pressure-area-temperature and energy relations of monolayers of octadecanitrile. l. Am. Chem. Soc., 64:1600. 1943 Intermolecular forces and two-dimensional systems. Publ. 21, Am. Assoc. Adv. Sci., p. 40. With G. Jura. A new adsorption isotherm which is valid over a very wide range of pressure. l. Chem. Phys., 11:430. With G. Jura. An absolute method for the determination of the area of a fine crystalline powder. l. Chem. Phys., 11:430. With G. aura. An adsorption method for the determination of the area of a solid without the assumption of a molecular area, and the area occupied by nitrogen molecules on the surfaces of solids. J. Chem. Phys., 11:431. With G. aura. The extension of the attractive energy of a solid into an adjacent liquid or film and the decrease of energy with distance. i. Chem. Phys., 1 1: 560. With G. aura. The relationship between the energy of adsorption of a vapor on a solid and of immersion of the solid in a liquid. J. Chem. Phys., 11:561. 1944 The surfaces of solids and liquids and the films that form upon them. I. Liquids. In: Colloid Chemistry, ed. by i. Alexander. New York: Reinhold Publishing Corporation. With G. Jura. The surfaces of solids and liquids and the films that form upon them. II. Solids and adsorption at the surfaces of solids or liquids. In: Colloid Chemistry, ed. by T. Alexander, vol. VI. New York: Reinhold Publishing Corporation. With G. Tura. The decrease of free surface energy as a basis for the development of equations for adsorption isotherms; and the existence of two condensed phases in films on solids. I. Chem. Phys., 12:1 12. With G. Jura. Surfaces of solids. X. Extension of the attractive energy of a solid into an adjacent liquid or film, the decrease of energy with distance, and the thickness of films. l. Am. Chem. Soc., 66:919.

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78 BIOGRAPHICAL MEMOIRS With G. Aura. Surfaces of solids. XI. Determination of the decrease of free surface energy of a solid by an adsorbed film. l. Am. Chem. Soc., 66: 1356. With G. aura. Surfaces of solids. XII. An absolute method for the determination of the area of a finely divided crystalline solid. i. Am. Chem. Soc., 66: 1362. With G. Jura. Surfaces of solids. XIII. A vapor adsorption method for the determination of the area of a solid without the assump- tion of a molecular area, and the areas occupied by nitrogen and other molecules on the surface of a solid. l. Am. Chem. Soc., 66: 1366. With G. aura. Equations for the pressure-area relations (isotherms) of liquid expanded and intermediate monolayers on water. J. Chem. Phys., 12:113. With G. Aura. The existence of expanded and intermediate phases in films on solids. l. Chem. Phys., 12:114. 1945 Determination of surface and interracial tension. In: Physical Methods of Organic Chemistry, ed. by A. Weissberger, vol. I. New York: Interscience Publishers, Inc. Determination of properties of monolayers and duplex films. In: Physical Methods of Organic Chemistry, ed. by A. Weissberger, vol. I. New York: Interscience Publishers, Inc. Surfaces of solids in science and industry. Science, 102:263. A general theory of the reaction loci in emulsion polymerization. J. Chem. Phys., 13:381. With G. Jura, E. H. Loeser, and P. R. Basford. A first order change which involves the vaporization in two dimensions of n-heptane on the surface of silver. l. Chem. Phys., 13: 535. 1946 The neutron, the intermediate or compound nucleus, and the atomic bomb. Science, 103:289. A general theory of the reaction loci in emulsion polymerization. II. J. Chem. Phys., 14:47. With R. W. Mattoon and M. L. Corrin. Structure of soap micelles indicated by x rays and the theory of molecular orientation. I. Aqueous solutions. J. Am. Chem. Soc., 68:220.

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WILLIAM DRAPER HARKINS 79 With R. W. Mattoon and M. L. Corrin. Structure of soap micelles as indicated by x rays and interpreted by the theory of molecular orientation. II. The solubilization of hydrocarbons and other oils in aqueous soap solutions. i. Colloid Sci., 1:105. With G. Aura and E. El. Loeser. Surfaces of solids. XVI. Adsorbed films of water and normal heptane on the surface of graphite. l. Am. Chem. Soc., 68:554. With G. Aura. The contact angle between water and a monolayer of egg albumin on glass as a function of film pressure. i. Colloid Sci., 1:137. With G. Aura. Surfaces of solids. XIV. A unitary thermodynamic theory of the adsorption of vapors on solids and of insoluble films on liquid subphases. l. Am. Chem. Soc., 68:1941. With G. Jura, E. H. Loeser, and P. R. Basford. Surfaces of solids. XV. First-order phase changes of adsorbed Elms on the surfaces of solids; the film of n-heptane on ferric oxide. l. Chem. Phys., 14: 117. With R. S. Stearns. Loci of emulsion polymerization: the diffusion of organic molecules from emulsion droplets through an aqueous phase into soap micelles. l. Chem. Phys., 14:214. With R. S. Stearns. Loci of emulsion polymerization: diffusion of organic molecules from emulsion droplets through an aqueous phase into polymer latex particles. i. Chem. Phys., 14:215. With M. L. Corrin and H. B. Klevens. The critical concentration for the formation of micelles as indicated by the absorption spectrum of a cyanine dye. l. Chem. Phys., 14:216. With G. Jura and E. H. Loeser. Surfaces of solids. XVII. A first- and second-order phase change in the adsorbed film of n-heptane on graphite. J. Chem. Phys., 14:344. With M. L. Corrin and H. B. Klevens. The determination of critical concentrations for the formation of soap micelles by the spectral behavior of pinacyanol chloride. J. Chem. Phys., 14:480. With M. L. Corrin. The effect of solvents on the critical concentra- tion for micelle formation of cationic soaps. [. Chem. Phys., 14:640. With M. L. Corrin. Determination of critical concentrations for micelle formation in solutions of cationic soaps by changes in the color and fluorescence of dyes. l. Chem. Phys., 14:641. With M. L. Corrin. Critical concentrations for micelle formation in mixtures of anionic soaps. l. Colloid Sci., 1:469.

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80 BIOGRAPHICAL MEMOIRS 1947 With M. L. Corrin. Determination of the critical concentration for micelle formation in solutions of colloidal electrolytes by the spectral change of a dye. I. Am. Chem. Soc., 69:679. With M. L. Corrin. The effect of salts on the critical concentration for the formation of micelles in colloidal electrolytes. l. Am. Chem. Soc., 69:683. A general theory of the mechanism of emulsion polymerization. i. Am. Chem. Soc., 69:1428. With R. W. Mattoon and R. S. Stearns. Structure for soap micelles as indicated by a previously unrecognized x-ray diffraction band. J. Chem. Phys., 15: 209. With R. S. Stearns, H. Oppenheimer and E. Simon. Solubilization by solutions of long-chain colloidal electrolytes. l. Chem. Phys., 15:496. With R. W. Mattoon and R. Mittelmann. A new type of micelle: soap with alcohol, amine or other polar-nonpolar molecules. J. Chem. Phys., 15: 763. 1948 A cylindrical model for the small soap micelle. l. Chem. Phys., 16: 156. With R. W. Mattoon and R. S. Stearns. Structure of micelles of colloidal electrolytes. III. A new long-spacing x-ray band, and the relations of other bands. J. Chem. Phys., 16:644. With H. Oppenheimer. A new type of micelle; solubility by film penetration. J. Chem. Phys., 16:1000. With P. R. Basford and G. Aura. Surfaces of solids. XVIII. The heats of immersion and desorption of water from graphite at 25. i. Am. Chem. Soc., 70:1444. 1949 With M. Popelka, Jr. The existence of stable nuclei as related to the principle of regularity and continuity of series and the ends of nuclear shells. Phys. Rev., 76:989. The effect of nuclear shells upon the pattern of the atomic species. Phys. Rev., 76:1538. With H. Oppenheimer. Solubilization of polar-nonpolar sub-

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WILLIAM DRAPER HARKINS 81 stances in solutions of long chain electrolytes. l. Am. Chem. Soc., 71:808. With R. Mittelmann. X-ray investigations of the structure of col- loidal electrolytes. IV. A new type of micelle formed by film penetration. l. Colloid Sci., 4:367. With R. Mittelmann and M. L. Corrin. Types of solubilization in solutions of long-chain colloidal electrolytes. l. Phys. Colloid Chem.,53:1350. With M. L. Corrin, E. L. Lind, and A. Roginsky. Adsorption of long-chain electrolytes from aqueous solution on graphite of known area and on polystyrene. I. Colloid Sci., 4:485. 1950 The intermediate-compound nucleus in nuclear reactions. In: Colloid Chemistry, ed. by I. Alexander, vol. VII. New York: Reinhold Publishing Corporation. Equivalence of protons and neutrons in nuclei. Phys. Rev., 78:634. Special and magic numbers as factors in nuclear stability and abundance. Phys. Rev., 79:724. With S. H. Herzfeld, A. Roginsky, and M. L. Corrin. Monomer- polymer ratio in emulsion polymerization of styrene. J. Polym. Sci., 5:207. General theory of emulsion polymerization. II. I. Polym. Sci., 5:217. Soap solutions: salt, alcohol, micelles, rubber. Sci. Mon., 70:220. With E. H. Loeser. Surfaces of solids. XIX. Molecular interaction between metals and hydrocarbons. J. Chem. Phys., 18:556. With E. H. Loeser. Surfaces of solids. XXI. Areas of nonporous solids from adsorption isotherms of n-heptane or n-hexane. l. Am. Chem Soc., 72:3427. With S. H. Herzfeld and M. L. Corrin. The effect of alcohols and of alcohols and salts on the critical micelle concentration of dodecylammonium chloride. I. Phys. Colloid Chem., 54:271. 1952 Physical Chemistry of Surface Films. New York: Reinhold Publish- ing Corporation. xvi + 413 pp.