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The Preston of the Guinier-Preston Zones. Guinier

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Abstract

Almost all materials scientists know about the Guinier–Preston (GP) zones, which were discovered in age-hardened aluminum-copper alloys in 1938. One of the discoverers, the French André Guinier, is rightly well known. The other discoverer, the British G.D. Preston, is totally ignored, even in English scientific biographies. I wish here to partly make up for this “oblivion” by giving elements about George Preston’s life (August 8, 1896 to June 22, 1972) and scientific work. Born in Ireland to the physicist Thomas Preston and deceased in Scotland, G. Preston carried out his scientific achievements in England, mainly studying the crystallographic structure of metals, metallic alloys, and thin films of metal oxides in a pioneering way. He also discussed the atomistic structure of twins in 1927. He mastered many kinds of X-ray and electron diffraction techniques up to diffuse scattering, which allowed him to detect the GP zones. Although he was involved in several controversies, including one about diamonds, he always remained a forthright person until his final professorship in Dundee. André Guinier’s career is briefly recalled in a parallel way.

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Notes

  1. Oundle School was founded in 1556 and is one of the largest independent schools in Great Britain; it occupies buildings throughout the small and attractive market town of Oundle located about 80 miles north of London.

  2. Officially recognized as a University in 1318 by Pope John XXII, the Cambridge institution was created after a violent “gown” vs “town” quarrel, which took place in Oxford in 1208 (or 1209) and led several Oxonian Scholars to flee the University of Oxford in search of a new location.

  3. Neither Peter Debye, being Dutch, nor Paul Scherrer, being Swiss, were affected by conscription.

  4. The casual challenge for Albert Hull was to determine the crystal structure of iron, which he thought might be a clue to the magnetic properties he was interested in at the General Electric Company. He had asked W. H. Bragg, who had solved the copper case, and Bragg answered him "We have tried but haven’t succeeded" (see References 7 and 8).

  5. Edgar Bain in the United States, at the Cleveland Wire Division of the General Electric Company, was bringing the first X-ray evidence[16,17] E. Bain proposed to translate the German Mischkrystalle (cristaux mixtes in French) by miscible crystals rather than mixed crystals.[18] His proposition has not been adopted.

  6. Dislocation in crystals was not yet known.

  7. E. Bain also studied Sn, Zn, Mg and Al in Cu; Cd and Zn in Ag; and W, Mo, Cr and Mg in Fe.[18]

  8. In 1923, Linus Pauling solved the structure of Mg2Sn in Pasadena,[20] and Gösta Phragmén worked out the structures of FeSi and Fe2Si in Stockholm.[21] Arne Westgren and G. Phragmén also worked on Cu-Zn, Ag-Zn, and Au-Zn alloys in 1925 and on CuZn, Cu3Al, and Cu5Sn compounds in 1926.[22,23]

  9. All this also illustrates a statement made by Georges Friedel in 1904: “Nous trouverons, au cours de l'étude des espèces, des raisons de croire que c'est le réseau matériel plutôt que le réseau cristallin des points analogues qui détermine les macles.”[36] (“We shall find, during the studies of species, reasons to believe that it is the atomistic lattice rather than the mathematical lattice which determines twins”).

  10. Being British, C. Desch would have written aluminium, with an i. But his book was printed in the United States. On this spelling issue, see the etymology section in en.wikipedia.org/wiki/Aluminium.

  11. This corresponds to Al-1.74 pct atoms Cu.

  12. The GP zones are truly nanoscopic objects.

  13. World War II was declared in Europe on the 3rd of September, two days after the invasion of Poland.

  14. In 1918, Faxén mainly introduced a more complete mathematical treatment with no easy to grasp physical hint.[59] Besides, he kept to Debye’s wrong ansatz about the use of the Born-von-Kàrmàn normal coordinates method, which was to be corrected in 1923 by Waller to give the correct Debye–Waller factor.[60]

  15. Quantification was introduced by Waller in 1925, 1928, Ott in 1935, and Born and Sarginson in 1941.

  16. R.W. James in 1954 stated that “It is hardly too much to say that an effect which for many years had been regarded as of secondary importance in comparison with the reduction of the intensity of the main maxima by thermal movement has now become that most likely to repay detailed study.”[61]

  17. Compare Reference 67 with Reference 68. I mainly agree with Rajinder Singh’s analyses, not on some factual statements.

  18. As Lonsdale stated in 1942, it is important to emphasize “that Laval discovered nearly all the major experimental facts concerning the extra reflections, and that he did so as the result of a well planned scheme of research.”[67] Jean Laval was then in prison in Germany. Kathleen Lonsdale could read French.

  19. Born in Norway in 1906, Willie Zachariasen had been hired by the Chicago University in 1930 and remained there for 44 years. He was given U.S. citizenship in 1941 in order to be allowed to work within the Manhattan project on the crystal chemistry of transuranium elements. Zachariasen died in 1979. His little book Theory of X-Ray Diffraction in Crystals (Wiley & Sons, 1945) is certainly worth reading.

  20. And had been knighted in 1929. Born, who was six years older than Raman, got his Nobel Prize only in 1954. G. Venkataraman stated it was globally wrong but locally correct. Indeed, as Born wrote in 1943, “Hence these acoustical branches are responsible for the infinite increase of scattering power in the vicinity of the reciprocal lattice points.” Léon Van Hove was to associate his name to these singularities using more sophisticated and general arguments 10 years later.[73]

  21. The classification is actually presently much richer, with types IaA, IaB, IaA/B, Ib, IIa, and IIb.

  22. A scientific account of the several Raman–Born controversies will require a whole article. Oddly enough, Jean Laval will be on Raman’s side in the early 1950s about the number of theoretically independent elastic constants (they got 45 instead of 21 in the triclinic case). Elastic constants can be measured via thermal diffuse scattering.

  23. The actual structure of these zones was essentially solved only many years later thanks to the combination of several experimental techniques and involves subtitutional and interstitial paired nitrogens for nitrogen-rich platelet models and tetranitrogen configurations surrounding carbon vacancies for nitrogen-low platelet models.

  24. Elected Fellow of the Royal Society of London in 1954, R. D. Preston has an extended biography in the Biographical Memoirs of the FRS (in 2005, by D. Cushing).

  25. Dundee is also famous for the Tay Bridge disaster, which occurred on December 28, 1879, when the first Tay Rail Bridge, which crossed the Firth of Tay between Dundee and Wormit collapsed during a violent storm while a train was passing over it. The conception of this bridge, by the just ennobled Sir Thomas Bouch, had been largely underestimated. Although the quality of the puddled iron was not faulty, this disaster did contribute to the establishment of the engineering subject of metallurgy as a proper academic subject of applied research and teaching.

  26. And Preston and Guinier never met.

  27. Preston may also have been a wine connoisseur; It is known that G. I. Finch used a wine bottle with the base cut off to house and insulate the electron gun of his electron diffraction chamber (the Finch camera) at Imperial College, London, in the 1930s. A Barsac bottle was preferred, according to George Preston (see Reference 82), who also built an electron diffraction apparatus for his studies of metal oxidation mentioned at the end of Section III–A.

  28. At his death, his name was given to a carrefour (crossroads) in the Forest of Fontainebleau near Paris. André Guinier’s grandfather, Ernest Guinier (1837–1908) spent his career in the Alps and the Pyrenees and contributed to lively debates on forestry from 1875 to 1900, many of which are still up to date.

  29. Founded in 1794 as the École normale de l’an III, it was rapidly closed to be ressuscitated by Napoléon in 1808 under another name. It was given back its original name in 1830, turned into École normale supérieure in 1845, and settled rue d’Ulm two years later.

  30. Founded in 1530 by François Ist, at the urging of the humanist scholar Guillaume Budé.

  31. Jean Calvet was the director of the Metallurgy Department of Joliot’s Laboratoire de Chimie Nucléaire. This department had recently been created, thanks to Frédéric Joliot. Pierre Armand Jacquet had joined Calvet as a researcher. Jacquet (1906–1967) patented in 1930/1 a method of electrolytic polishing (electrolytic polishing actually hacks back to Georges Charpy in the early 1890s), thanks to which the metallographic micrographs were considerably improved because the surface of the sample is not perturbed as after mechanical polishing. Calvet and Jacquet had hoped to be able to see Merica’s “knots” in age-hardened aluminum-copper alloys, but they could not see anything at that stage.

  32. Because of a miswriting in his civil birth act, R. Castaing had to officially spell his first name as Raimond, with an i, once he became a Member of the Academy of Sciences in 1977.[91]

  33. The accidental death of their son Daniel that same year deeply affected André Guinier and his wife.

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  94. A. Guinier: Théorie et Technique de la Radiocristallographie, Dunod, Paris, France, 1956 and 1965 (susbstantially augmented versions of Radiocristallographie, Dunod, Paris, France 1945 but without Mauguin’s preface. Ch. Mauguin, who died in 1958, was too feeble to write an updated preface. The 1956 edition was translated by P. Lorrain and D. Lorrain: X-Ray Diffraction in Crystals, Imperfect Crystals, and Amorphous Bodies, Freeman, San Francisco, CA, 1963. Radiocristallographie was translated by T.L. Tippett, and edited by K. Lonsdale with a foreword by K. Lonsdale: X-Ray Crystallography Technology, Hilger and Watts, London, UK, 1952.).

  95. A. Guinier and G. Fournet: Small Angle Scattering of X-Rays, translated by C.B. Walker, Wiley, New York, NY, 1955.

  96. M. Lambert: “André Guinier, un des «pères fondateurs» de notre Université,” Orsay-Infos, 2000, vol. 61, p. 14.

  97. M. Lambert: “André Guinier,” Acta Crystallographica A, 2001, vol. 57, pp. 1–3.

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  98. R. Comès: “André Guinier (1911–2000),” J. Physique, 2002, vol. 12, pp. 1–6.

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  99. B. Jouffrey: “Hommage à André Guinier, Membre de l’Institut,” Revue Métallurgie-CIT/SGM, 2002, vol. 2, pp. 95–96.

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  100. A. Guinier: “Personal Reminiscences,” in Fifty Years of X-Ray Diffraction, Ed. P.P. Ewald, International Union of Crystallography, Utrecht, The Netherlands, 1962, pp. 574–78.

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  101. A. Guinier: “On the Birth of GP Zones,” Mater. Sci. Forum, 1996, vols. 217–222, pp. 3–6.

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  102. A. Guinier: “As Chance should have it…,” Rigaku J., 1999, vol. 16, p. 2.

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Here are some additional publications by G.D. Preston, which I read but did not include in the main text

  1. E.A. Owen and G.D. Preston: “The Effect of Rolling on the Crystal Structure of Aluminium,” Proc. Phys. Soc. London, vol. 38, London, UK, 1925, pp. 132–47.

  2. E.A. Owen and G.D. Preston: “X-Ray Tube with Detachable Electrodes Suitable for Crystals,” J. Sci. Instrum., 1926, vol. 4, pp. 1–3.

  3. G.D. Preston, with Marie L.V. Gayler: “Exhibits Relating to the Crystal Structure of Manganese and of Aluminium Alloys,” Proc. Phys. Soc., 1929, vol. 41, pp. 590–91.

  4. G.D. Preston: “Age-Hardening of Copper-Aluminium Alloys,” Proc. Phys. Soc., 1940, vol. 52, pp. 77–79. (+ Discussions, pp. 94–101).

  5. G.D. Preston: “Diffuse Reflexion of X-Rays,” Nature, 1941, vol. 147, pp. 358–59.

  6. G.D. Preston: “Precipitation in the Solid State,” J. Sci. Instrum. (London), 1941, vol. 18, pp. 154–57.

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Acknowledgments

I thank Professor Sandy Fitzgerald, who retired recently from the Harris Chair of Physics at Dundee; Stephen Forge, Archivist of Oundle School where Preston studied as a young boy; and Ms. Sylvia Chantler from the NPL Library and Information Services. An obituary was published in The Times, on June 29, 1972. I also wish to thank the library departments of the École Polytechnique and of the CEA Saclay. Last, but not least, I also wish to thank Professor David Brandon for quite a few scientific and historical discussions.

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  1. Laboratoire des Solides Irradiés, École Polytechnique, 91128, Palaiseau Cedex, France

    O.B.M. Hardouin Duparc (Senior Researcher)

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Correspondence to O.B.M. Hardouin Duparc.

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This article is a significantly enlarged version of a paper I wrote in French in 2001.[1]

Manuscript submitted May 11, 2010.

Appendices

Appendix A: The Strange Fate of The Prestons

G.D. Preston is not mentioned as such in the French Encyclopædia Universalis or in the Encyclopædia Britannica, the C.C. Gillispie Dictionary of Scientific Biography (1970–1981), the Biographical Encyclopedia of Scientists (1994), or in the Cambridge Dictionary of Scientists (1996). His father Thomas Preston, was in the 1943–1974 printed version of the Enc. Brit. but disappeared in the 2001 CD version. Such a complete oblivion seems a pity, both for the Prestons and for the history of science.

Robert Cahn depreciated Preston in his obituary for André Guinier[83]: “Guinier’s paper [in Nature[46]] was followed immediately by another written by a Briton, G.D. Preston. A close examination of that second paper clearly shows that Preston must have been a referee for Guinier’s contribution, and that he then rushed into print in order to share primacy of discovery.” Cahn thought Preston behaved unethically. I hope I succeeded in convincing him of the contrary when I sent him my French article[1] in 2005 (he knew French, see Reference 84) and in subsequent e-mail exchanges.

A very similar story actually occurred only a few months before, in the January 8th issue of Nature 1938 about the discovery of superfluid helium, with an article by P. Kapitza followed immediately by another written by two Britons, J.F. Allen and A.D. Misener on pages 74-5, see the story detailed by Balibar.[85]

In his history-oriented book, The Coming of Materials Science,[86] Cahn wrote “independent observations by Guinier (1938) in France and Preston (1938) in Scotland” Yet, in 1938, Preston was in England, at NPL. In a more recent book, one can even read that R. Preston discovered the basic phenomenon in the United States and was killed during World War II (sic).[87]

Appendix B: A Few Words On André Guinier

André Jean Guinier was born the August 1, 1911, in Nancy, as son and grandson of respected foresters. His father, Philibert Guinier (1876–1962), wrote more than 200 papers and several books and may be considered as a pioneer of ecology in France.Footnote 28

André Guinier so brilliantly followed the prestigious École Normale Supérieure in ParisFootnote 29 that he was allowed to choose his thesis adviser in 1936. He chose the crystallographer Charles Mauguin who asked him to study the X-ray scattering outside the Bragg-Laue diffraction spots. This scattering, much less intense than the Bragg scattering, is called diffuse scattering. It is not random, however, and it translates, in the reciprocal space, all that is neither perfect crystalline order nor complete homogeneous disorder. Examples are disorder due to thermal agitation in crystals (thermal diffuse scattering), due to local distortion of the crystalline parameter in the vicinity of a defect (structural diffuse scattering), and also due to the presence of particles randomly dispersed in a homogeneous matrix, even an amorphous one. Mauguin had already observed structural diffuse scattering on black mica (biotite) sheets.[88] Besides the problem of the correct interpretation of the diffuse scattering, the difficulty also was to be able to detect it with sufficient accuracy. As a compromise between these two difficulties, Guinier focused his attention to the experimental and theoretical study of SAXS (sometimes also called the “Guinier domain”). He designed and realized a high precision microbeam monochromatic X-ray camera, the principle of which is now famous under the name of “Guinier camera.”[89] He first applied it to the successful determination of the sizes of the small colloidal particles (10 Å to 100 Å) thanks to a theoretical formula he established, which is called the Guinier formula or Guinier law.[90] In order to still improve the quality of his camera, André Guinier went to ask for aluminum sheets to two excellent metallurgists who were working at the Collège de France,Footnote 30 Jean Calvet and Pierre Jacquet.Footnote 31 While discussing with them about their respective works, he realized that his camera could be used to check the hypothesis, which was proposed to explain the structural hardening of the aluminum copper alloys with a few percents of copper in mass, namely the presence of microprecipitates (or, should we now better say, nanoprecipitates) of copper in the hardened alloys. Indeed, such objects, if they really existed, as most metallurgists believed, were too small to be directly detected by the tools available at that time (Jacquet had tried and failed) but ought to give a detectable signal in diffuse scattering, at least in the small-angle domain. André Guinier immediately achieved diffraction photographs with his camera and got specific streaks, which proved the validity of the hypothesis. He could even give information about the shape and size of these nanoprecipitates—small disks of copper atoms gathered in {100} planes of the (face centered cubic) aluminum matrix.

André Guinier was starting his scientific career and went on to use the SAXS technique to investigate the rich field of imperfections in crystals and materials for several decades. Besides his scientific career, André Guinier founded, with Raymond Castaing (1921–1999)Footnote 32 and Jacques Friedel, the Laboratoire de Physique des Solides in Orsay in 1959.Footnote 33

He was a great teacher, who also wrote several books of high-quality popularization,[92,93] besides his classical Théorie et Technique de la Radiocristallographie.[94] He wrote his famous Small Angle Scattering of X-Rays with Gérard Fournet.[95] André Guinier died in Paris on July 3, 2000. Professors Marianne Lambert, Robert Comès, and Bernard Jouffrey wrote obituaries in French and in English,[96–99] and so did Robert Cahn.[84] On several occasions, Guinier has given his own reminiscences about the birth of the GP zones.[100–102]

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Hardouin Duparc, O. The Preston of the Guinier-Preston Zones. Guinier. Metall Mater Trans B 41, 925–934 (2010). https://doi.org/10.1007/s11663-010-9387-z

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