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Biographical Memoirs: Volume 62

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Biographical Memoirs: Volume 62 JOEL HENRY HILDEBRAND November 16, 1881-April 30, 1983 BY KENNETH S. PITZER THIS BIOGRAPHICAL SUMMARY differs from that for a typical scientist in many respects. First, there is the remarkable diversity of fields in which Joel Hildebrand made major contributions. To research scientists and engineers, his contributions to our knowledge of liquids and nonelectrolyte solutions are most important. But a substantially larger group recognize him as their outstanding teacher of freshman chemistry and often as the most inspiring teacher of their college experience. Others know him as mountaineer, lover of the outdoors, president of the Sierra Club, and coauthor with his daughter Louise of a charming little book, Camp Catering. There was his effective leadership in a variety of educational and scientific organizations far beyond chemistry, involving service as a member of the Council of the National Academy of Sciences (1949-52), dean of men and dean of the College of Letters and Science at the University of California, and member of the Citizens Advisory Committee on Education to the California Legislature. And, finally, he continued his active professional life past age 101. It is a special pleasure to me to have the opportunity to write this biography. I first met Joel Hildebrand when I entered graduate school at Berkeley in 1935. His cordial-

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Biographical Memoirs: Volume 62 ity to young people was immediately apparent. Although I did not do my thesis research with him, I did consult him frequently and the discussion was always helpful. With my appointment to the faculty, the association with Joel continued and expanded to a wide range of activities and to personal friendships including our families—with mine of the generation of his children. Joel Henry Hildebrand was born on November 16, 1881, in Camden, New Jersey. His ancestors came to America before the revolution from the upper Rhine valley. When asked about his longevity, Joel replied, "I chose my ancestors carefully" and frequently added that most, if not all, lived well past eighty. His father, Howard Onid Hildebrand, was in the insurance business near Philadelphia, and Joel attended local schools. His intellectual interests were particularly stimulated by a grandfather who, although of limited schooling, had read widely and accumulated an excellent library. With his interest in natural phenomena aroused, Joel acquired and studied Dana's Geology, Newcomb's Astronomy, and similar books. After his high school mathematics was completed with solid geometry and trigonometry, he discovered independently the power and beauty of calculus. After he had learned as much chemistry as his teacher (the principal) knew, he was given the key to the laboratory, a college laboratory manual, and encouragement to learn more on his own. Joel told with justified pride about his experiment proving that nitric oxide gas was NO rather than N2O2—a result that demolished a theory in a book by a Harvard professor that he had been given. It is clear that this high school principal was a great source of encouragement also for opening to Joel broader horizons of interest in various cultural areas, including music. Hildebrand entered the University of Pennsylvania in 1899 and wisely chose a double major in chemistry and

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Biographical Memoirs: Volume 62 physics in the College of Arts and Science rather than a more "professional" course in chemistry that emphasized recipes for analysis and similar details. He thereby had the opportunity to learn not only more physics but also history, literature, and mathematics while avoiding details of chemistry that were unimportant and sometimes even untrue. After receiving his Ph.D. in 1906 in chemistry at Pennsylvania, Hildebrand was encouraged to spend a postdoctoral year in Germany learning the new science of physical chemistry before returning to teach it. He went to Berlin, where he attended lectures by J. H. van't Hoff and by Walter Nernst. He also did some research under Nernst and then returned to the University of Pennsylvania to serve on its faculty until 1913. In that year Gilbert N. Lewis invited Hildebrand to join the remarkable group of young chemists whom he selected and led in transforming the Chemistry Department at the University of California into a center of international eminence. Hildebrand's doctoral thesis of 1906 was entitled "The Determination of Anions in the Electrolyte Way," and he continued with several papers on electrochemical methods in analysis. Herbert S. Harned was his first research student, and Harned's thesis was in this area. But Hildebrand soon shifted his primary interests to physical rather than analytical topics (as did Harned, who proceeded to a very distinguished career at Yale and was elected to the National Academy of Sciences). The color of iodine solutions fascinated Hildebrand throughout his career; his first paper on that topic, "Uber die Farbe von Jodlosungen," was published in 1910. He soon noted (1920) that the deviations from Raoult's law of various violet solutions of I2 formed a regular pattern. However, the curve for I2 in benzene differed from this pattern, and the solution had a somewhat different color. This color differ-

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Biographical Memoirs: Volume 62 ence suggested a more intimate interaction of the iodine with benzene. These ideas were extended in many directions through the years. The concept of a regular pattern of positive deviations from Raoult's law grew into a general theory of ''regular solutions." Such systems involve no specific solvation or association and the mixing of their molecules is essentially random. Equations for the activities of the components of such solutions had already been developed by several scientists, but these suffered either from the absence of relationships to the properties of the pure components or, in van Laar's case, to making these connections through an approximate equation of state. While the van der Waals equation was a great advance at the time and it gives a reasonable representation of gas imperfection, the quantitative deviations in the liquid region are large, and it is the liquid region that is pertinent to liquid solutions. Scatchard published a paper in 1931 which, in his words, "may be regarded as a quantitative development of the treatment of Hildebrand, although it disagrees with his ideas in some important details, or as a method of freeing the van Laar treatment from the inadequacies of the van der Waals equation." Hildebrand and Wood derived the same equation two years later by a very different and modern method—by integrating the intermolecular pair potentials throughout the liquid weighted by the radial distribution function. Both Scatchard's and Hildebrand's results yield the same working equation relating the deviation from ideal solutions (Raoult's law) to the cohesive energy density of the pure components, that is, ΔE/ V, where E is the energy of vaporization of a volume V of the pure liquid. More precisely, it is the square of the difference in the square roots,

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Biographical Memoirs: Volume 62 [(E1/ V>1 )1/2-(E2/ V2)1/2] 2, that determines the departure from ideality. In recent years, this quantity, (E/V)1/2, has been called the solubility parameter (or Hildebrand's solubility parameter) and given the symbol δ. The Scatchard-Hildebrand equation is quite successful—better than any other equation of comparable simplicity and generality. But it is not surprising that there are departures from perfect agreement, and from time to time Hildebrand presented tables of adjusted solubility parameters that yield improved agreement. These are always discussed in relation to aspects of the intermolecular forces that might explain the need for adjustment. Joel's effort to improve the theory of regular solutions continued with a final paper in 1979. Hildebrand, always the effective teacher, summarized the current status of knowledge about nonelectrolyte solutions in monographs designed to interest and instruct chemists. Initially, these were general reports on the status of knowledge in the field and carried the title The Solubility of Nonelectrolytes. The successive editions of 1924, 1936, and 1950 (the last with R. L. Scott) grew in size along with the rapid advance of knowledge in this area. Opposite the title page of the third edition is a picture of a tube containing seven incompletely miscible liquids (heptane, aniline, water, perfluorokerosene, phosphorus, gallium, and mercury)—a beautiful example of Joel's flair for generating interest in and enjoyment of his topic for discussion. After 1950, Joel left to others the task of general review of knowledge concerning nonelectrolyte solutions, and he prepared smaller books concentrating on the areas of his particular interest. These were Regular Solutions in 1962 with R. L. Scott and Regular and Related Solutions: The Solubility of Gases, Liquids, and Solids in 1970 with J. M. Prausnitz and R. L. Scott.

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Biographical Memoirs: Volume 62 The relationship of the color of iodine solutions to their other characteristics was noted. Joel maintained a continuing interest in the changes of color (or new spectral features) as an indication of bonding. The one case where I was coauthor with Joel of a published paper arose from a series of discussions in this general area; it is entitled "Color and Bond Character" and appeared in 1941. Hildebrand's most important discovery in this area came in a series of papers with H. A. Benesi in 1949-50 that related an intense ultraviolet absorption to the formation of electron donor-acceptor complexes. This type of complex, now more commonly called a charge-transfer complex, has been investigated extensively by others, is well understood theoretically, and is an integral part of our body of organized knowledge. The "rule" that carries the Hildebrand name concerns the entropy of vaporization of a normal liquid. In 1915 he showed that, for a typical group of "normal" liquids boiling near or below room temperature, the entropy of vaporization was more nearly constant if compared at a constant vapor volume rather than on the constant pressure basis of Trouton's rule. With this considerably higher precision of agreement, the Hildebrand rule became a much more useful criterion of a normal liquid. In comparison, hydrogen-bonded or other highly polar liquids have larger entropies of vaporization than do "normal" liquids. Another idea of Hildebrand's that has great practical as well as theoretical importance concerns the use of helium in deep diving. A diver at depth experiences high pressure and correspondingly increased solubility of breathing gases in his blood. The problem of the "bends"—the release of this gas as a bubble in a blood passage when the diver emerges—was well known. In the mid-twenties Hildebrand suggested that this problem could be ameliorated by substituting helium for nitrogen in mixture with

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Biographical Memoirs: Volume 62 oxygen for the diver's breathing gas. Not only is the solubility of helium much less than that of nitrogen at a given pressure, but also the diffusion rate is faster. These basic ideas have had a major role in improving diving capability and safety ever since. Also in the mid-twenties, Hildebrand initiated precise physical-chemical studies of anhydrous hydrogen fluoride and fluorine. Among other studies, he and Simons measured the anomalous P-V-T behavior of HF and interpreted it on a polymerization basis. Simons proceeded from this beginning to a fruitful career of specialization in fluorine chemistry. Through the years Joel took pleasure in demolishing concepts that he regarded as spurious or misleading. He was not fooled by "polywater." He was severely critical of theories of liquids that were based on complex assumptions about structural features for which there was no direct verification. With the deeper insight of molecular dynamics calculations, these complex assumptions have now been disproved in many cases. But Joel had refused to accept these theories, even if they were reasonably successful in representing the experimental data available at the time. Several of these situations are described in his 1977 paper, "Operations on Swollen Theories with Occam's Razor." Another case of this type is the "hydrophobic effect" or, worse, the "hydrophobic bond." Joel objected to these terms because "phobic" implies repulsion. It is true that in aqueous solution a solute containing both alkyl (or other non-polar) groups and polar groups will arrange itself in a manner to favor water contact with the polar groups of the solute and alkyl group contact with other alkyl groups. But this does not mean that an alkyl group is actually repelled by a water molecule. Rather, as Hildebrand concludes, "There is no hydrophobia between water and alkanes; there is only

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Biographical Memoirs: Volume 62 not enough hydrophilia to pry apart the hydrogen bonds of water so that the alkanes can go into solution without assistance from attached polar groups." In the period 1970-77 Joel gave considerable attention to the viscosity of liquids or, as he preferred, the fluidity that is the reciprocal of viscosity. These papers are collected in a small monograph, Viscosity and Diffusivity: A Predictive Treatment, published in 1977 with an introduction by J. O. Hirschfelder. In the introduction Hirschfelder writes of Hildebrand, "Somehow, he has the ability to sweep away all of the complexities and discover simple relationships which will take theoreticians another generation to derive." Indeed, Joel often presented new empirical relationships that were simpler and more accurate than those in common use. And he presented them in a simple qualitative theoretical framework that was free from inconsistencies or the complexities often contrived to circumvent inconsistencies. This book often elicited the comment that "Hildebrand is a genius in finding ways to present data so that they fall on a straight line." But Joel's were not merely functions yielding straight lines; he also required conformity to general ideas of molecular structure and behavior. Indeed, he was a genius in research of this type. Hildebrand's impact as a teacher was just as important and in many respects more remarkable than his role in research. His freshman chemistry lectures, given regularly from 1913 until his "retirement" in 1952, were legendary. Thousands of alumni recall his vivid descriptions and dramatic demonstrations as well as his enlivening digressions into music, art, and mountaineering. A single course was offered at Berkeley with total enrollment usually somewhat over 1,000, with lectures in a room seating about 500, but with laboratory, quiz, and discussion in groups of twenty-five. William Bray and Wendell

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Biographical Memoirs: Volume 62 Latimer (both members of the Academy) took primary responsibility for the laboratory and wrote the book for it. Most of the regular faculty supervised freshman sections (in addition to other teaching) and thereby initiated the graduate students into their teaching assistant duties in an apprenticeship pattern. Thus, there was extensive involvement of most of the faculty with the general chemistry course and general agreement concerning its character. But Hildebrand gave the lectures, wrote the quizzes and examinations, and was in general charge of the course. He also wrote the central text, Principles of Chemistry, which was revised several times. The course at Berkeley, as developed by Hildebrand, Bray, Latimer, and others, departed from the pattern of that time by much greater emphasis on principles, with reduced attention to memory of specific factual material. It was only after about twenty-five years that other textbooks began to appear that reflected a similar emphasis. Of course, the "Berkeley" books were used elsewhere in the intervening years. As is often the case, the pattern has recently shifted farther (probably too far) toward dominance of theory and general principles and the near exclusion of "factual" material. The "Hildebrand" course maintained a balance; the student learned that, while important aspects of chemistry could be related to general principles through relatively simple equations, other experimental facts were best remembered, if important enough, or looked up when needed. To promote the habit of quick and convenient reference to this body of knowledge, Latimer and Hildebrand prepared their Reference Book of Inorganic Chemistry (1928). It was revised several times and was available combined with Principles of Chemistry in a single volume. Joel was superb as a lecturer and thoroughly enjoyed it. There were many lecture experiments with an entertaining

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Biographical Memoirs: Volume 62 aspect and lots of humorous comments that the students enjoyed. But Joel never lost sight of the primary purpose of the lectures, and most of these entertaining features were tied into the primary lesson of the day. Joel's enthusiasm, combined with thorough knowledge and excellent lecture technique, was almost irresistible. There was never a problem of slack attendance at Hildebrand lectures. From 1913 through 1952, Hildebrand had about 40,000 students in his freshman lectures. While only a moderate proportion followed chemistry professionally, many became engineers, physicists, or other scientists. Others became lawyers, business executives, and leaders in various fields, and they have a clearer picture of the role of science in the modern world because of their contact with Joel Hildebrand. His impact as a teacher was great indeed. This fame as a teacher of chemistry gave Joel the credentials and brought invitations to influence educational matters more broadly. His former students, now in a multitude of positions of responsibility and influence, urged his inclusion on committees, boards, and conferences. A notable example was the Citizens Advisory Committee to the Joint Education Committee of the California legislature. Joel had all of the qualifications of a good administrator or organizational leader. He never shirked such responsibilities when they were pressed upon him, but he never let such duties draw him permanently away from his primary interests in teaching and research. His preferences in this respect fitted very comfortably with the policies of the University of California, wherein academic administration was in the hands of distinguished professors, but there was no implication that a given individual would continue indefinitely as a department chairman or a dean. Indeed, the status of ex-dean was most highly regarded at the Berkeley Faculty Club.

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Biographical Memoirs: Volume 62 1933 With S. E. Wood. The derivation of equations for regular solutions. J. Chem. Phys. 1:817-22. With G. R. Negishi and L. H. Donnally. Solubility XIII. The solubility of iodine in certain solvents. J. Am. Chem. Soc. 55:4793-4800. 1934 With W. H. Claussen. The vapor pressure of fluorine. J. Am. Chem. Soc. 56:614-15. With W. H. Claussen. The vapor pressures of hydrogen and deuterium fluorides. J. Am. Chem. Soc. 56:1820. Complex formation due to polarization. J. Chem. Phys. 2:822-23. 1935 Solubility. XIV. Experimental tests of a general equation for solubility. J. Am. Chem. Soc. 57:866-71. 1936 Dipole attraction and hydrogen bond formation in their relation to solubility. Science 83:21-24. With W. E. Morrell. The distribution of molecules in a model liquid. J. Chem. Phys. 4:224-27. Thermodynamic aspects of the theory of non-electrolytic solutions. Chem. Rev. 18:315-23. With G. R. Negishi. The heat of fusion and vapor pressure of stannic iodide. J. Am. Chem. Soc. 58:2293. Solubility of Non-Electrolytes, 2nd ed. New York: Reinhold. 1937 Intermolecular forces in solutions. Trans. Faraday Soc. 33:144-51. (Introductory paper at the General Discussion on "Structure and Molecular Forces in a) Pure Liquids and b) Solutions," Sept. 1936.) With G. R. Negishi. Solubility. XV. The solubility of liquid and solid stannic iodide in silicon tetrachloride. J. Am. Chem. Soc. 59:339-41. The validity of Raoult's law for paraffin molecules of very different length. J. Am. Chem. Soc. 59:794-98. With S. E. Wood. Deviations of carbon tetrachloride and silicon tetrachloride solutions from Raoult's law. J. Am. Chem. Soc. 59:1510.

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Biographical Memoirs: Volume 62 With R. D. Vold. A calorimetric test of the solubility equation for regular solutions. J. Am. Chem. Soc. 59:1515-21. The incomplete solubility of liquid iodine in carbon tetrachloride. J. Am. Chem. Soc. 59:2083-85. 1938 With Louise Hildebrand. Camp Catering. Brattleboro, Vt.: Stephen Daye Press. With K. S. Frederick. Specific heats and heat of fusion of iodine. J. Am. Chem. Soc. 60:1436-39. With K. J. Frederick. Specific heats and heat of fusion of tellurium tetrachloride. J. Am. Chem. Soc. 60:2522-23. 1939 Liquid structure and energy of vaporization. J. Chem. Phys. 7:1-2. Several solutions of non-polar substances. J. Phys. Chem. 43:109-17. With J. W. Sweny. The entropy of solution of hexane with hexadecane. J. Phys. Chem. 43:297-300. Liquid structure and entropy of vaporization. J. Chem. Phys. 7:233-35. Order and disorder in pure liquids and solutions. Science 90:1-8. (William H. Nichols Medal Address.) With K. J. Frederick. Specific heats and heats of fusion and transition of carbon tetrabromide. J. Am. Chem. Soc. 61:1555-58. With R. N. Boyd and H. R. R. Wakeham. The effect of temperature on the structure of mercury . J. Chem. Phys. 7:458-62. With H. R. R. Wakeham and R. N. Boyd. The intermolecular potential of mercury. J. Chem. Phys. 7:958-62. 1941 With K. S. Pitzer. Color and bond character. J. Am. Chem. Soc. 63:2472-75. Emulsion type. J Phys. Chem. 45:1303—5. 1942 With F. E. Young. The heat of fusion and the heat capacities of solid and liquid white phosphorus. J. Am. Chem. Soc. 64:839-40. 1943 With R. W. Long and W. E. Morrell. The polymerization of gaseous hydrogen and deuterium fluorides. J. Am. Chem. Soc. 65:182-7.

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Biographical Memoirs: Volume 62 With J. A. Campbell. The structure of liquid mercury. J. Chem. Phys. 11:330-33. With J. A. Campbell. The structure of liquid xenon. J. Chem. Phys. 11:334-37. 1944 The liquid state. Proc. Phys. Soc. (London) 56:221-39. (Guthrie Lecture for 1944.) Abstract in Nature (London) 154:227. 1946 A reaction velocity with large negative temperature coefficient. J. Am. Chem. Soc. 68:915. 1947 With A. R. Olson. An unusual liquid interface. J. Phys. Colloid Chem. 51:567-68. The entropy of solution of molecules of different size. J. Chem. Phys. 15:225-28. With T. S. Gilman. Comments on the Hildebrand Rule. J. Chem. Phys. 15:229-31. Forces between polyatomic molecules. Proc. Natl. Acad. Sci. U.S.A. 33:201-4. Forces between tetrahalide molecules. J. Chem. Phys. 15:727-36. 1948 The Lowdown on Higher Education. Stanford, Calif.: James Ladd Delkin. With A. Gee. Relative association of hydrogen and deuterium fluorides in the liquid state. J. Am. Chem. Soc. 70:427-28. With H. A. Benesi. Ultraviolet absorption bands of iodine in aromatic hydrocarbons. J. Am. Chem. Soc. 70:2832-33. With C. Groot. The solubility relations of white phosphorus. J. Am. Chem. Soc. 70:3815-18. With H. A. Benesi. Solubility of iodine in 1,2- and 1,1-dichloroethanes, cis-and trans-dichloroethylenes and perfluoro-n-heptane. J. Am. Chem. Soc. 70:3978-81. 1949 With D. R. F. Cochran. Liquid-liquid solubility of perfluoromethylcyclohexane with benzene, carbon tetrachloride, chlorobenzene, chloroform and toluene. J. Am. Chem. Soc. 71:22-25.

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Biographical Memoirs: Volume 62 A critique of the theory of solubility of non-electrolytes. Chem. Rev. 44:37-45. With A. Wachter. The solubility of n-dotriacontane (dicetyl). J. Phys. Colloid Chem. 53:886. On an interpretation of the solubility of organic compounds in water. J. Phys. Colloid Chem. 53:973. A philosophy of teaching. J. Chem. Educ. 26:450. (Remson Lecture.) With H. A. Benesi. A spectrophotometric investigation of the interaction of iodine with aromatic hydrocarbons . J. Am. Chem. Soc. 71:2703-7. With J. C. Gjaldbaek. The solubility of nitrogen in carbon disulfide, benzene, normal- and cyclo-hexane, and in three fluorocarbons. J. Am. Chem. Soc. 71:3147-50. With H. A. Benesi. Interaction of iodine with aromatic hydrocarbons. Nature (London) 163:963. Solubility of water in hydrocarbons. J. Chem. Phys. 17:1346. 1950 Factors determining solubility among non-electrolytes. Proc. Natl. Acad. Sci. U.S.A. 36:7-15. With J. C. Gjaldbaek. The solubility of chlorine in normal perfluoroheptane and other liquids. J. Am. Chem. Soc. 72:609-11. With H. A. Benesi and L. M. Mower. Solubility of iodine in ethyl alcohol, ethyl ether, mesitylene, p-xylene, 2,2-dimethylbutane, cyclohexane, and perfluoro-n-heptane. J. Am. Chem. Soc. 72:1017-20. With J. C. Gjaldbaek. On some partial molal volumes of gases in solution. J. Am. Chem. Soc. 72:1077-78. With H. A. Benesi. The absorption spectrum of iodine in acetone. J. Am. Chem. Soc. 72:2273. An irregularity in the solvent powers of paraffins. J. Chem. Phys. 18:1337-38. With B. B. Fisher and H. A. Benesi. Solubility of perfluoro-n-heptane with benzene, carbon tetrachloride, chloroform, n-heptane and 2,2,4-trimethylpentane. J. Am. Chem. Soc. 72:4348-51. With R. L. Scott. Solutions of nonelectrolytes. Annu. Rev. Phys. Chem. 1:75-92. With R. L. Scott. The Solubility of Nonelectrolytes, 3rd ed. New York: Reinhold.

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Biographical Memoirs: Volume 62 1951 With G. J. Rotariu. Supercooling of liquid phosphorus. J. Am. Chem. Soc. 73:2524-25. With R. E. Powell and T. S. Gilman. Crystallization velocity of liquid phosophorus. J. Am. Chem. Soc. 73:2525-26. With G. J. Rotariu, E. Schramke, and T. S. Gilman. The solubility of mercury in liquid phosphorus. J. Am. Chem. Soc. 73:2527-28. Nine or more liquid phases. J. Am. Chem. Soc. 73:5008. 1952 The temperature dependence of the solubility of solid nonelectrolytes. J. Chem. Phys. 20:190-91. With G. J. Rotariu. Some applications of solubility theory to analytical problems. Anal. Chem. 24:770-73. With G. J. Rotariu and E. W. Haycock. The solubility of water in liquid phosphorus. J. Am. Chem. Soc. 74:3165-66. Solubility relations of fluorocarbons. Chem. Eng. Prog. Symp. Ser. 48(3):39. With G. J. Rotariu. Molecular order in n-heptane and n-perfluoroheptane. J. Am. Chem. Soc. 74:4455-56. With R. L. Scott. The entropy of solution of nonelectrolytes. J. Chem. Phys. 20:1520-21. The ''critical point." J. Colloid Sci. 7:551-52. With G. J. Rotariu and D. W. Fraga. The solubility of water in normal perfluoroheptane. J. Am. Chem. Soc. 74:5783. 1953 With G. Jura, D. Fraga, and G. Maki. Phenomena in the liquid-liquid critical region. Proc. Natl. Acad. Sci. U.S.A. 39:19-23. With E. W. Haycock and B. J. Alder. The diffusion of iodine in carbon tetrachloride under pressure. J. Chem. Phys. 21:1601-4. Models and molecules. Discuss. Faraday Soc. 15:9-23. (Seventh Spiers Memorial Lecture.) 1954 With B. J. Alder, E. W. Haycock, and H. Watts. PVT relations of liquid carbon tetrachloride and n-perfluoroheptane and a test of the Clausius-Mosotti equation. J. Chem. Phys. 22:1060-61. A simple correlation of gas solubilities. J. Phys. Chem. 58:671-72. With B. J. Alder, J. W. Beams, and H. M. Dixon. The effects of

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Biographical Memoirs: Volume 62 hydrostatic pressure and centrifugal fields upon critical liquid-liquid interfaces. J. Phys. Chem. 58:577-79. 1955 With G. J. Rotariu and D. W. Fraga. The density of n-octane and 2,2,3,3-tetramethylbutane at low temperatures. J. Phys. Chem. 59:187. With H. Watts and B. J. Alder. Self-diffusion of carbon tetrachloride, isobars and isochores. J. Chem. Phys. 23:659-61. 1956 With D. N. Glew and L. W. Reeves. Purification of perfluoro-n-heptane and perfluoromethylcyclohexane. J. Phys. Chem. 60:615. With D. N. Glew. The solubility and partial molal volume of iodine in perfluoro-n-heptane. J. Phys. Chem. 60:616-18. With D. N. Glew. The entropy of solution of iodine. J. Phys. Chem. 60:618-20. With L. W. Reeves. The entropy of solution of bromine in perfluoro-n-heptane. J. Phys. Chem. 60:949-52. 1957 Science in the Making. (The Bampton Lectures in America.) New York: Columbia University Press. With L. W. Reeves. The solubility and entropy of solution of argon in five selected nonpolar solvents. J. Am. Chem. Soc. 79:1313-14. With K. Shinoda. The solubility and entropy of solution of iodine in octamethylcyclotetrasiloxane and tetraethoxysilane. J. Phys. Chem. 61:789-91. With J. E. Jolley. The liquid-liquid solubility of octamethylcyclotetrasiloxane with perfluoromethylcyclohexane and perfluoro-n-heptane . J. Phys. Chem. 61:791-93. 1958 With J. E. Jolley. Solubility, entropy and partial molal volumes in solutions of gases in non-polar solvents. J. Am. Chem. Soc. 80:1050-54. With K. Shinoda. The solubility and entropy of solution of iodine in n-C7F16, c-C6F11CF3, (C3F7COOCH2)4C, c-C4Cl2F6, CCl2FI=CCIF2, and CHBr3. J. Phys. Chem. 62:292-94. With K. Shinoda. Partial molal volumes of iodine in various complexing and non-complexing solvents. J. Phys. Chem. 62:295-96. With K. Shinoda. Liquid-liquid solubility of pentaerythritol

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Biographical Memoirs: Volume 62 tetraperfluorobutyrate with chloroform, carbon tetrachloride and octamethylcyclotetrasiloxane. J. Phys. Chem. 62:481-83. 1959 With H. Schmidt and G. Jura. The heat capacity of the system carbon tetrachloride-perfluoromethylcyclohexane through the critical region. J. Phys. Chem. 63:297-99. With E. B. Smith and J. Walkley. Intermolecular forces involving chlorofluorocarbons. J. Phys. Chem. 63:703-4. With J. Walkley. Partial vapor pressure and entropy of solution of iodine. J. Phys. Chem. 63:1174. With E. B. Smith. Liquid isochores and derived functions of n-C7F1 6, c-C6F11CF3, c-C4Cl2F6, n-2,2,3C4Cl3F7, CCl2FI=C-Cl2F, and CCl4. J. Chem. Phys. 31:145-47. With J. Walkley. Partial molal volumes of hydrogen and deuterium. J. Am. Chem. Soc. 81:4439. Free volumes in liquids. J. Chem. Phys. 31:1423-25. 1960 With E. B. Smith and J. Walkley. Correlation of solubility relations of stannic iodide, iodine, sulfur, and phosphorus. Trans. Faraday Soc. 56:220-24. The entropy of solution of iodine at constant volume. J. Phys. Chem. 64:370-71. With J. Walkley and D. N. Glew. Relations between ultraviolet and visible absorption peaks of iodine solutions. J. Chem. Phys. 33:621-22. With E. Smith and J. Walkley. The partial molal volume and entropy of solution of stannic iodide. Trans. Faraday Soc. 56:1276-80. 1961 With K. Shinoda. Compressibilities and isochores of (C3F7COOCH2)4C, c-Si4O4(CH3)8, n-C5H12, n-C8H18, 2, 2,4-C5H9(CH3)3, c-C5H10, cC6H12, c-C6H11 CH3, C6H5-CH3, p-C6H4(CH3)2 s-C6H3(CH3)3, CH2Cl2. J. Phys. Chem. 65:183. With Y. Kobatake. Solubility and entropy of solutions of He, N2, A, O2, CH4, C2H6, CO2 and SF6 in various solvents; regularity of gas solubilities. J. Phys. Chem. 65:331-35. With K. Shinoda. Critical composition in liquid mixtures of components of very different molal volumes. J. Phys. Chem. 65:1885-86.

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Biographical Memoirs: Volume 62 With R. Fujishiro and K. Shinoda. Partial molal volumes in liquid-liquid mixtures. J. Phys. Chem. 65:2268-69. With G. Archer. Evidence regarding liquid structure. Proc. Natl. Acad. Sci. U.S.A. 47:1881-82. 1962 With R. L. Scott. Regular Solutions. Englewood Cliffs, NJ.: Prentice-Hall. With R. Fujishiro. The liquid-liquid solubility of cyclohexane and perfluorotributylamine at 25°. J. Phys. Chem. 66:573. 1963 Is Intelligence Important? New York: Macmillan. An Introduction to Molecular Kinetic Theory—Selected Topics in Modern Chemistry. New York: Reinhold. With H. Eyring and S. Rice. The liquid state. Int. Sci. Technol. (15):56-66. With H. Hiraoka. Solubility relations of the isomeric trichlorotri-fluoroethanes. J. Phys. Chem. 67:916-18. With M. Ross. Energy volume relations of octamethylcyclotetrasiloxane and its mixtures with carbon tetrachloride. J. Phys. Chem. 67:1301-3. With L. W. Reeves. The solubility of carbon tetrafluoride in perfluoromethylcyclohexane. J. Phys. Chem. 67:1918. With G. Archer. The solubility and entropy of solution of carbon tetrafluoride and sulfur hexafluoride in nonpolar solvents. J. Phys. Chem. 67:1830-33. With H. Hiraoka. Partial molal volumes of sulfur hexafluoride. J. Phys. Chem. 67:1919. Prefatory chapter: Fifty years of physical chemistry in Berkeley. Annu. Rev. Phys. Chem. 14:1-4. 1964 Intermolecular forces between molecules of different species. J. Chem. Phys., 61:53-57. With H. Hiraoka. The solubility and entropy of solution of certain gases in (C4F9)3N, CCl2Fl=CClF2, and 2,2,4-(CH3)3C5H9. J. Phys. Chem. 68:213-14. With E. B. Smith. Further evidence concerning liquid structure. J. Chem. Phys. 40:909-10. With M. Ross. Diffusion of hydrogen, deuterium, nitrogen, argon, methane and carbon tetrafluoride in carbon tetrachloride. J. Chem. Phys. 40:2397-99.

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Biographical Memoirs: Volume 62 With K. Shinoda. Mutual solubility of perfluoroheptane with carbon tetrachloride and carbon disulfide at 25°. J. Phys. Chem. 68:3904-5. The use of models in physical science. Proc. Am. Philos. Soc. 108:411-17. (Reprinted in Scuola Azione, 1965, 1:18-35 (in Italian).) 1965 With K. Shinoda. Irregular solutions of iodine. J. Phys. Chem. 69:605-8. With K. Nakanishi and E. M. Voigt. Quantum effect in the diffusion of gases in liquids at 25°C. J. Chem. Phys. 42:1860-63. With J. Dymond. Effect of methyl groups upon the solvent power of aliphatic liquids. Proc. Natl. Acad. Sci. U.S.A. 54:1001-3. 1966 With E. M. Voigt. Charge-transfer spectra in nonpolar solvents. J. Phys. Chem. 70:598-600. 1967 With J. Dymond. Partial molal volumes in regular solutions. J. Chem. Phys. 46:624-26. With J. Dymond. Attractive potentials between fluorochemicals and aliphatic hydrocarbons. J. Phys. Chem. 71:1145-47. With J. Dymond. An apparatus for accurate, rapid determinations of the solubility of gases in liquids. Ind. Eng. Chem. Fundam. 6:130-31. With J. H. Dymond. The solubility of a series of gases in cyclohexane and dimethylsulfoxide. J. Phys. Chem. 71:1829-31. With T. Soda. Solubility of iodine in dimethyl sulfoxide. J. Phys. Chem. 71:4561-63. 1968 With K. W. Miller. Solutions of inert gases in water. J. Am. Chem. Soc. 90:3001-4. With K. W. Miller. The solubility of fluorocarbon gases in cyclohexane. J. Phys. Chem. 72:2248-49. With E. M. Voigt. Absorption maxima of the visible band of iodine in different groups of solvents. J Phys. Chem. 72:3300-5. 1969 With R. G. Linford. Partial molal volumes of fluorochemical gases in cyclohexane. Trans. Faraday Soc. 65:1470-72.

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Biographical Memoirs: Volume 62 With R. G. Linford. Calculation of partial from total vapor pressures: System-C6H6 + CCl2Fl=CClF2. Ind. Eng. Chem. Fundam. 8:846-47. With R. G. Linford. Solubility of gases in mixtures of nonpolar liquids. J. Phys. Chem. 73:4410-11. Relative diffusivities of methane in water and carbon tetrachloride. Proc. Natl. Acad. Sci. U.S.A. 64:1329-30. Thermodynamic parameters for dissolved gases. Proc. Natl. Acad. Sci. U.S.A. 64:1331-34. 1970 With J. M. Prausnitz and R. L. Scott. Regular and Related Solutions—The Solubility of Gases, Liquids, and Solids. New York: Van Nostrand Reinhold. With R. G. Linford. Solubility and entropy of solution of gases in CCl2Fl=CClF2. Trans. Faraday Soc. 66:577-81. With R. G. Linford and R. J. Powell. A comparison of the Gibbs energy and entropy of interfaces water-n-hexane and waterper-fluorotributylamine. J. Phys. Chem. 74:3024-25. 1971 Motions of molecules in liquids: viscosity and diffusivity. Science 174:490-93. With R. J. Powell. Diffusivity of He3, He4, H2, D2, Ne, CH4, Ar, Kr, and CF4 in (C4F9)3N. J. Chem. Phys. 55:4715-16. 1972 With R. J. Powell. Solubility of 16 gases in (C4F9)3N and CS2. J. Chem. Eng. Data 17:302-4. With R. H. Lamoreaux. Fluidity: A general theory. Proc. Natl. Acad. Sci. U.S.A. 69:3428-31. 1973 With R. H. Lamoreaux. Fluidity and liquid structure. J. Phys. Chem. 77:1471-73. With B. J. Alder. Activation energy: Not involved in transport processes in liquids. Ind. Eng. Chem. Fundam. 12:387-88. 1974 With R. H. Lamoreaux. Fluidity along continuous paths between liquid and gas. Physica 74:416-22.

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Biographical Memoirs: Volume 62 With R. H. Lamoreaux. Solubility of gases in liquids: fact and theory. Ind. Eng. Chem. Fundam. 13:110-15. With R. H. Lamoreaux. Diffusivity of gases in liquids. Proc. Natl. Acad. Sci. U.S.A. 71:3321-24. With R. H. Lamoreaux. Diffusivity of methane in a mixture of CCl4 and c-C6F11C2F5 of the critical composition in the region above the temperature of separation. Proc. Natl. Acad. Sci. U.S.A. 71:3800-3801. 1975 Kinetic theory of viscosity of compressed fluids. Proc. Natl. Acad. Sci. U.S.A. 72:1970-72. 1976 With R. H. Lamoreaux. Viscosity of liquid metals: an interpretation. Proc. Natl. Acad. Sci. U.S.A. 73:988-89. Viscosity of dilute gases and vapors. Proc. Natl. Arad. Sci. U.S.A. 73:4302-3. 1977 Viscosity and Diffusion—A Predictive Treatment. New York: Wiley. 1978 Viscosity of dilute gases and vapors of polyatomic molecules. Mol. Phys. 35:519-23. With B. J. Alder, W. E. Alley, and J. W. Beams. Effect of centrifuging on fluctuations in the critical liquid-liquid region. J. Chem. Phys. 68:3099-3102. Theories and facts about liquids. Discuss. Faraday Soc. 66:151-59. Brilliant total reflection from a liquid-liquid interface. Proc. Natl. Acad. Sci. U.S.A. 75:5772. Absence of outer non-bonding electrons in methyl groups affects solubility parameters. Ind. Eng. Chem. Fundam. 17:365-66. 1979 An improvement in the theory of regular solutions. Proc. Natl. Acad. Sci. U.S.A. 76:6040-41. 1981 With R. H. Lamoreaux and A. G. Loomis. The state of hydrogen in liquid metals. High Temp. Sci. 14:51-54. A history of solution theory. Annu. Rev. Phys. Chem. 32:1-23.