Dr. B. Pfeiffer GSI Helmholtzzentrum für Schwerionenforschung

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1 Dr. B. Pfeiffer GSI Helmholtzzentrum für Schwerionenforschung Seminar für Kern- und Kosmochemie (“K&K Seminar”) MPI für Chemie, Mainz, Mittwoch, 10.2.2010, 17:15 alances from “De re me- allica, Liber Septem” . Agricola, 1556 Atomic Mass Evaluations Contributions of the Kaiser-Wilhelm-/Max-Planck- Institut für Chemie Mass spectrograph built at Kaiser-Wilhelm Institut für Chemie in 1943 Motivation: scientific and personal Importance of balances for rebirth of atomic hypothesis around 1800 Prout‘s hypothesis Isotopes Contributions from Kaiser-Wilhelm- Institut für Chemie AMEs at Max-Planck-Institut Future AME

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Atomic Mass Evaluations Contributions of the Kaiser-Wilhelm-/Max-Planck- Institut für Chemie. Dr. B. Pfeiffer GSI Helmholtzzentrum für Schwerionenforschung. Motivation: scientific and personal Importance of balances for rebirth of atomic hypothesis around 1800 Prout‘s hypothesis - PowerPoint PPT Presentation

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Dr. B. PfeifferGSI Helmholtzzentrum für Schwerionenforschung

Seminar für Kern- und Kosmochemie (“K&K Seminar”)MPI für Chemie, Mainz, Mittwoch, 10.2.2010, 17:15

Balances from “De re me-tallica, Liber Septem” G. Agricola, 1556

Atomic Mass EvaluationsContributions of the Kaiser-Wilhelm-/Max-Planck-

Institut für Chemie

Mass spectrograph built atKaiser-Wilhelm Institut fürChemie in 1943

• Motivation: scientific and personal• Importance of balances for rebirth of atomic hypothesis around 1800 • Prout‘s hypothesis• Isotopes• Contributions from Kaiser-Wilhelm- Institut für Chemie• AMEs at Max-Planck-Institut• Future AME

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Pre-history of talk, personal motivation

In summer during a „Nachsitzung“‡, Prof. Palme mentioned to have seen a mass spectro-graph at the MPI. It had once been in the group of Mattauch. I remembered that he had published mass evaluations together with A.H. Wapstra. It was proposed to ask G. Audito give a seminar on the collaboration of the Mainz group with Wapstra. But he got incontact with Wapstra only 20 years later and so I was „made volunteer“ for a talk.

Some days later, I remembered my early days at the II. Physikalisches Institut in Gießen.In a cellar, there had been a very old mass spectrograph built by the director Prof. Ewaldlong ago. I vaguely had in mind that he had been in connection with Mattauch. Sudden-ly arose the suspicion that Prof. Palme might have seen this apparatus in Mainz.

So I started to search for clues to the history of this spectrograph and to the relation between Ewald and Mattauch. Browsing through data bases as diverse as GOOGLEand the NASA/Harvard Astrophysical Base I surprisingly found some publications ofEwald together with Mattauch, Hahn, Strassmann going back to around 1940.There were also hints to the wartime activities in the „Uranverein“, but I would like tohave more serious sources before discussing these topics.

Just in December, I was recalled that Ewald liked to put some students in his car whenhe attended the early GSI seminars in Darmstadt-Wixhausen.

‡ C. Burkhard, 1.7.09

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GSI 1972

Very early days of GSI

?

In the December 2009 issue of target, the scientific magazine of GSI, is displayed a picture from the early days of GSI (not yet atthe actual site). Prof. Ewald is easy to identify. I am not surewho is the young guy at the left. It could be myself.

Courtesy Prof. Rudolf Bock

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“Prehistory” of atomic weights

The atomic hypothesis of Leukippos and Demokritos was never forgotten,but the Four-Element theory of Empedokles was the mainstream for 2 millenia.Alchemy was mainly concerned with qualitative attributes of substances, quantitative analysis was performed by craftsmen in the mints or ore mines (see, e.g. G. Agricola: De re metallica libri XII, 1556).

Modern chemistry is interested in quantitative relations between elements:Influenced by neoplatonic philosophy, J.B. Richter introduced 1792 „chymisches Rechnen“, in scientific notation stoichiometry. ’Anfangsgründe der Stöchyometrie oder Meßkunst chymischer Elemente’.

To disprove his teacher Bertholet, J.L. Proust established 1799 the “Law of Definite Proportions”, which was modified by J. Dalton’s “Law of Multiple Proportions”.

In order to explain these chemical laws Dalton re-introduced the atomic hypothesis, inspired by his studies of the physical laws of gases.

From Liber Septimus

For this audience, I need not explain the scientific motivation for determining atomic masses. But the physicists in this field tend to oversee that the importance of mass did not start with the detection of isotopes at the beginning of the 20th century!

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Illustrations to various editions of Thomas Norton‘s Ordinall of Alchemy (ca. 1477)

I started the search reading that alchemists weremerely interested in „quality“ not quantity. Prof. H.Gebelein, a modern alchemist, shows the figure atthe right side above. He is convinced of the transmutation of elementsby alchemy, not only by atom smashers and neutrons.

Alchemists and balances

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Dokumastic in the Scripture?

Jeremias, 6 ca. 600 B.C.E.

Zechariah, 13 after 500 B.C.E.

Ezekiel, 22 ca. 580 B.C.E.

29: The bellows are burned, the lead is consumed of the fire; the founder melteth in vain: for the wicked are not plucked away.30: Reprobate silver shall men call them, because the LORD hath rejected them.

9: And I will bring the third part through the fire, and will refine them as silver is refined, and will try them as gold is tried: they shall call on my name, and I will hear them: I will say, It is my people: and they shall say, The LORD is my God.

17: And the word of the LORD came unto me, saying, 18: Son of man, the house of Israel is to me become dross: all they are brass, and tin, and iron, and lead, in the midst of the furnace; they are even the dross of silver. 19: Therefore thus saith the Lord GOD; Because ye are all become dross, behold, therefore I will gather you into the midst of Jerusalem. 20: As they gather silver, and brass, and iron, and lead, and tin, into the midst of the furnace, to blow the fire upon it, to melt it; so will I gather you in mine anger and in my fury, and I will leave you there, and melt you. 21: Yea, I will gather you, and blow upon you in the fire of my wrath, and ye shall be melted in the midst therof. 22: As silver is melted in the midst of the furnace, so shall ye be melted in the midst thereof; and ye shall know that I the LORD have poured out my fury upon you.

The first explicit reference to this analytical tool is in Pliny the Elder: Historia Naturalis.

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This led to stoichiometry and the proportio-nal laws. Based on these principles, 1868/9D.I. Mendeleev and L. Meyer developed then the Periodic System of the Elements.

Over time, the (al)chemists had discovered more than the 4 (5) classical “elements“.They were a “hermetically sealed” community and their cryptic works are difficult to understand and often their names stand for compounds or even more general principles:• “antimony“ was Stibnit (Sb2S3), • the element Sb was known as “antimony regulus“ The first task for modern chemistry was to find an unequivocaldefinition of “element”, as already requested by Robert Boyle 1661.

Decisive was the shift from “quality“ to “quantity“,

the use of precise balances.

Part of texts on astrology or alchemy?

Basis for the periodic system of the elements

The upcoming of a rudimentary chemical „industry“ with the need of fixed proceduresinstead of philosophical theories lead tomodern chemistry:

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Table of the relative weights of the ultimate particles of gaseous and other bodies

Appended toJ. Dalton“On the Absorption of Gases by Water and Other Liquids”Memoirs and Proceedings of the Manchester Literary and Philosophical Society, Manchester, 1805, vol. 6, pp. 271-287

http://web.lemoyne.edu/~giunta/dalton52.html

This paper was already presented orally in 1803.It contains the first steps to the atomic hypothesisto explain the laws of definite and multiple pro-portions.The first table of relative weights is appendedwithout explanation of the methods applied.

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John DaltonA New System of Chemical Philosophy (1808)

http://www.archive.org/stream/newsystemofchemi01daltuoft

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10http://www.us.archive.org/GnuBook/?id=newsystemofchemi01daltuoft#0

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New Tableof the relative weights of atoms

J. Dalton, A New System of Chemical Philosophy, Manchester,printed by the executors of S. Russell for George Wilson, London, 1827, vol. 2, p. 352

Remark:Dalton, contrary to most fellow chemists,was convinced that two atoms of the same element cannot be part of a mole-cule. Therefore, his reference mass for hydrogenin reality is 0.5.His formula for water is HO instead of H2O, etc. Avogadro obtained forN 13.238 instead of 13.8964 O 15.074 “ 15.8734in units of H=1.

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“On the relation between the specific gravities of bodies in their gaseous state and the weights of their atoms” Annals of Philosophy 6 (1815) 321

“Correction of a mistake in the essay on the relation between the specific gravities of bodies in their gaseous state and the weights of their atoms” Annals of Philosophy 7 (1816) 111http://web.lemoyne.edu/~giunta/PROUT.HTML#prout2

L. Meinecke, “Das specifische Gewicht der elastischen Flüssigkeiten” Annalen der Physik 24 (1816) 159

Prout-(Meinecke)-hypothesis

In 1816, the physician Prout (and the chemist L. Meinecke) put forward the hypothesis that all relative weights of the elements are whole-number multiples of the weight of hydrogen.[It is generally assumed, that he did not base this assumption on contemporary measurements, but on natural philosophy. He set the πρωτη νλη of the Greek philosophers synonymous with H.]

In the following decades, chemists pushed the techniques to the limits in order to prove or disprove Prout’s hypothesis (and advanced many ad-hoc “improvements”).Around 1860, relative atomic weights for 57 elements had been determined andthey were one essential ingredient for the establishment of the “Periodic System” by Mendeleev and Meyer.

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An ahead of time nucleosynthesis hypothesis?

Some scientists in the 19th century assumed that “atoms” were composed of H atoms (and a glue).

Does anyone know, if someone may have speculated on “nucleosynthesis” by adding H on atoms?

Or was their believe in the creation as described in Genesis unshakeable? Especially, as “atomists” were regarded as irreligious atheists. ‡

Physician William Prout1785-1850

And was the discovery of natural radioactivity really so surprising at the end of acentury in which Prout‘s hypothesis had been discussed all time?

J.J. Thomson mentioned Prout when he presented his model of the atom: an about1 Ǻ diameter elastic ball, in which electrons were imbedded.

‡ The referee for Gregor Mendel’s heredetary laws turned down the publication as he regarded it as “atomistic”.

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Platon influenced Prout, Crookes (prot(o)yle), Gamow (hylem).1919 Ernest Rutherford proved that nuclei of hydrogen are contained in other elementsas theorized by Prout. He named it to honour Prout. Someauthors assume that he was influenced by Crookes’ “protyle”, other that it is coined after“Prout”.

In the mid thirteenth century encyclopædia Liber de proprietatibus rerum of Bartholomaeus Anglicus, Platois quoted as describing the hyle, ,the “primary matter”, in the following terms:

Platon’s influence on modern science

“Hyle was without quantity, without quality, without colour,without kind, without place, and without time,something that was not matter and yet not absenceof matter”

The encyclopædist then continued: “These words are not easy to fathom.”

L.M. Celnikier: Find a hotter place! A History of Nuclear Astrophysics.

Christ in midst of the 4 elementsFirst english print by Wynken de Worde, Westminster,1495

πρωτη νλη

„το πρωτον“ (the first),

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Testing Prout’s hypothesis

Jan Servais Stas (1813-1891)Jean-Charles-Galissard de Marignac

(1817-1894)

Prout’s hypothesis was accepted bymost scientists, and had followerstill the end of the century despite contrary evidence. More precise measurements were performed as by J. J. Berzelius (1828) or J.-B. Dumas. Most discon-certing was the value for chlorine: ~35.5. Some proposed, that the basic unit was ½ the weight of H (and then ¼and 1/8 ….).

Many casted doubt on the measurement techniques, especially the purity of the samples (which often was correct). This forced the chemists to bring to perfection their methods.Stas and de Marignac disproved the hypothesis. They determined the atomic weightsof 57 elements, laying the basis for the Periodic System of the Elements. In 1861, Sir W. Crookes had discovered thallium with the spectroscopic method. In 1870he undertook to determine the atomic weight with a carefully prepared measurement.

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Against oll odds!

W. Crookes: "Research on the Atomic Weight of Thallium"Proc. Roy. Soc. of London, Vol. 20 (1871-1872) pp. 475-483

The 2005 value for the element Tl is 204.383.300 ± 200 μu (in units of 12C/12).

Crookes applied Oelem/16 introduced by Stas.His result in these units could be 203.650.000 ± 2.200 μM.E.

All instruments were specially produced for this measurement.New technical developments were initiated, as for vacuumpumps.

It seems to me that Sir Crookes was somehow “disappointed”of the result:

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Modern values

Isotope Mass [μu] Multiples of 1H

1H 1008664.9157 ± 0.0006 203Tl 202972344.2 ± 1.4 201.2287205Tl 204974427.5 ± 1.4 203.2136

Elem. Isotop. compos. Mass [u] Multiples of H

H 99.9885%/0.0015% 1.000794(7)

C 98.9%/1.07% 12.0107(8) 12.0012

O 99.757%/0.038%/0.205% 15.9994(3) 15.9867

Tl 29.5%/70.5% 204.3833(2) 204.2212

ATOMIC WEIGHTS OF THE ELEMENTS 2005

(IUPAC TECHNICAL REPORT)Prepared for publication by M. E. WIESER

Pure Appl. Chem., Vol. 78, No. 11, pp. 2051–2066, 2006

http://www.iupac.org/publications/pac/2006/pdf/7811x2051.pdf

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Can one save Prout’s hypothesis?

In the second half of the 19th century, the new analytical method of spectroscopy was applied by some scientists to prove that atoms contained substructures. Leadingproponents were the chemist Crooke and the astrophysicist Norman Lockyer.Their ideas did not survive further scrutiny. Faint spectral lines, which they took forprove of substructures, were often indications to (trace) impurities in their samples.

Lockyer‘s concepts at least gave J.J. Thomson arguments for his theory that the atomcontained electrons.In literature, Crooke is often cited as precursor of the concept of isotopes.

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• The physician William Prout postulated in 1815 that all atomic weights are multiples of hydrogen.• Sir William Crookes hypothesized 1886 that deviations from this rule indicate to “isotopes“. • J.J. Thomson / F.W. Aston observed 1912 with cathode rays, that Ne had two isotopes of mass 20 and 22.• After the war, F.W. Aston measured isotopic masses (1919).• Based on these masses, Arthur Eddington explained 1926 the energy source of stars as fusion of H to He.

Atomic masses

Many isotopes were not accessible to experiments so thattheoretical mass formulas were developed. Based on the liquid drop modelC.F. v. Weizsäcker [Z. Physik 96 (1935) 431] andH.A. Bethe and R.F. Bacher [Rev. Mod. Phys. 8 (1936) 82]

developed a semiempirical mass formula, that served as basis for nucleosynthesis models for a long time, as the CNO- or Bethe-Weizsäcker-cycle:C.F. v. Weizsäcker, Z. Physik 39 (1938) 633 andH. Bethe, Phys. Rev. 55 (1939) 434

Hans Bethe1906-2005

Carl Friedrich vonWeizsäcker 1912 - 2007

Discovery of isotopes

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Dempster’s mass spectrometer

Dempster's 1918 mass spectrometer

Dempster, A. J. (1918). "A New Method of Positive Ray Analysis". Phys. Rev. 11: 316–325.

Arthur Jeffrey Dempster(1886 - 1950)

Na and K with low resolution

This rather simple design with a 180° magnetic sector field was used by many groups (but with important ameliorations!). The theoretical resolution was100 (with d=10 cm, slits .5 mm). This spectrum for Na and K had a resolution of 35 with 2 mm slit settings.

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From the beginning, the study of the new phenomenon radioactivity was performed at the institute. In 1918, p.e., Hahn and Meitner codiscovered 231Pa. The nuclear chemistry culminated 20 years later in the discovery ofnuclear fission. Many (all?) topics of interest at the MPI had already been studied in Berlin-Dahlem, as isotope geology including dating of rocks, isotopic abundances, atomic weights, extinct radio-activity. Mass spectroscopy was applied as a tool by the group of Mattauch, often in close collaboration with the nuclear chemists.

Kaiser-Wilhelm-Institut für Chemie

Kaiser-Wilhelm-Institut für Chemie – heute Otto-Hahn-Bau der Freien Universität Bild: FU Inauguration 28.10.1913

Built 1943 for an accelerator

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Isotopenberichte

Isotopenbericht, Tabellarische Übersicht der Eigenschaften der Atomkerne, soweit bis 1948 bekannt, von Prof. Dr. J. Mattauch und Doz. Dr. A. Flammersfeld. Sonderheft der Zeitschrift für Naturforschung, Verlag der Z. Naturforschung, Tübingen 1949, 243 S., 85 Abb., kartoniert DM 30.- (p 179)

Kernphysikalische Tabellen: mit einer Einführung in die Kernphysik J. Mattauch, S. Flügge, 1942This compilation includes tables of properties of isotopes as decay modes and masses. It was reprintedseveral times, mostly without authorisation, even after superior data were available.

The Kaiser-Wilhelm-Institut für Chemie published nearly every year “Isotopen-Berichte” with relevant results from groups all over the world.

G.T. Seaborg, I. Perlman: Table of Isotopes, Reviews of Modern Physics, vol. 20, Issue 4, pp. 585-667 were made available as manuscript and could be included.

Since 1940, the report was published also in Physikalische Zeitschrift, as the content hadshifted to physical methods.

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Combined compilations / evaluations

The major part in reality is the Introduction into Nuclear Physics, the tables are anappendix.In the case of the masses of the (ground states) of isotopes, the results of two “groups” are listed: - on the one hand the mass spectroscopists and - on the other the reaction people, who had problems with each other.

As an example, Mattauch published in 1942this booklet with lists of mass doublets and reaction Q-values and estimated masses up tothe actinides. In his Isotopic Report of 1949, masses are only derived up to mass 41, he regarded the reaction values as too uncertain.

Now, NUBASE combines masses of ground and long-lived isomeric states with halflives, spins and parities.

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Packing fraction curve 1938Following Aston, nuclear structure effects were represented by the „Packing fraction curve“. f = 10000 * (M-A)/A

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Packing fraction curve 1940

The „Berichte“ always contained the mostrecent „Packungsanteilkurve“.

For the lightnuclides, differentcurves aredrawn foreven and oddmass.

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Isotopic ratios and elemental atomic weight of Cu

H. Ewald, ZfP 122 (1944) 487

In 1944, no precision values for the isotope ratiosof Cu were known. Ewald not only measured theratio, but derived a new value for the atomic weight of Cu from this ratio.

The 2005 value is 63.546(3) u or 63,566 M.E.in agreement with the international value of 1944.

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Isotope geology, early Solar System

Zeitschrift für Physik 120 (1943) 598

Mattauch et al. repeated a measurement of W. Wahl from Helsingfors (Finland) and attributed the M=132 line to C11, instead to 132Ba from extinct 132Cs.Wahl insisted and Mattauch would have liked to invite Wahl to Berlin to repeatthe analysis with the original samples of Pollucit. But it was war time!

Walter August Wahl(1879 - 1970)

Pollucit(Cs,Na)2Al2Si4O12 • H2O

T1/2 of 132Cs was unknown in the early 1940‘s.

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Ewald’s double-focusing spectrograph

Heinz Ewald designed a double-focusing mass spectrograph at the Kaiser-Wilhelm-Institut in the years 1942 – 1944. It accompanied him in all his career and ended at theII. Physikalisches Institut in Gießen. There I saw it as a young student in a dark cellar.Now it is displayed more openly.Gottfried Münzenberg believes that it was once in Mainz. It had a mass resolution of>30.000. The MPI wanted to build the “ultimate” machine with a resolution of 100.000,but the design was flawed. Gottfried told me that parts for this instrument also had beenin the dark cellar in Gießen.

Heinz Ewald16.6.1914 –

5.2.1992

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Partly personal remarks on Heinz Ewald

     

H. Ewald u. H. Hintenberger: Methoden und Anwendungen der Massenspektroskopie; Weinheim : Verl. Chemie, 1953

H. Ewald: Die Analyse und Deutung der Neodymsalzspektren Annalen d. Physik. Folge 5, Bd 34, H. 3.; Göttingen, Math.-naturwiss. Diss., 1939

In war time, Ewald (+ Walcher + v. Ardenne) worked on electromagnetic isotope separa-tors for 235U. The Ardenne/Ewald plasma sources were more efficient than the americanones for the calutrons.

Later-on as director of II. Physik. Inst. in Gießen, he was engaged in the construction of LOHENGRIN, OSTIS and SHIP.

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Proposal of Ewald for an isotope separator 1942

Addendum 1:

Recently, R. Karlsch put forward the hypothesis that the German scientists had made substantial progress on the way to the atomic bomb. In Ewald/Hintenberger is shown a proposal for an isotope separator by Ewald 1942.In M. Walker „German National Socialism and the Quest for Nuclear Power 1939-1949“ is reported, that M. von Ardenne picked-up the idea and constructed a proto-type in his laboratory.

Prof. Schmidt-Rohr presumes that Ardenne built a full-fledged separator with the „Forschungsanstalt der Deutschen Reichspost“ in a circular bunker near Bad Saarow south of Berlin. This bunker corresponds to the one constructed for a cyclotron at Miersdorf.

http://www.petermann-heiko.de/index.php?option=com_content&view=article&id=83&Itemid=96&lang=de

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Addendum 2:

W. Walcher had built an isotope separator at Kiel, which allowed to separate p.e.some ten µgs of the stable Rb isotopes.

He was also involved in the „Uranverein“.

Recycling of a separator magnet

Z. Phys. 108, 376 (1938)

Around 1980, the magnet was used tobuilt the HELIOS-separator at the TRIGA reactorin Mainz:

A. K. Mazumdar, H. Wagner, G. Kromer, W. Walcher,M. Brügger, E. Stender, N. Trautmann and T. Lund;Nucl. Instr. and Meth. 174 (1980) 183

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Mattauch-Herzog type double-focusing spectrograph

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Mass doublets

12CH – 13C

12CH3 – 15N

4410 ± 8 μM.E. 4409 ± 9 μu 4470.185 ± 0.008 μu AME03

22317 ± 15 μM.E. 23310 ± 15 μu23366.1979 ± 0.0017 μu AME03

M.E. 16O/16u 12C/12M.E./1.0003179 = u

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Mass measurements for 13C and 15N

16O/16 12C/1213C 13,0079 ± 0,0002 (13,0038 ± 0,0002) Bainbridge 1936

13,00761 ± 0,00015 (13,00348 ± 0,00015) Livingston 1937

13,00758 ± 0,00006 (13,00345 ± 0,00006) Hahn 1940

13,007581 ± 0,000025 (13,003447 ± 0,000025) Ewald 1946

13,007478 ± 0,000005 (13,003344 ± 0,000005) Wapstra 1955

13,0074883 ± 0,0000007 13,0033543 ± 0,0000007 Everling 1960

13,00335483 ± 0,000000001 AME03

15N 15,0050 ± 0,0003 (15,0002 ± 0,003) Bainbridge 1936

15,00489 ± 0,00020 (15,00012 ± 0,00020) Livingston 1937

15,00494 ± 0,00007 (15,00017 ± 0,00007) Hahn 1940

15,004934 ± 0,000030 (15,000165 ± 0,000030) Ewald 1946

15,004862 ± 0.000005 (15,000093 ± 0,000005) Wapstra 1955

15,0048769 ± 0,0000009 15,0001081 ± 0,0000009 Everling 1960

15,00010889 ± 0,000000007 AME03

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Development of mass measurements

What happened between 1948 and1955?

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Why differs the value for 13C from the modern value?

fH fC-12

1940 81,31 3,243

1946 81,30 3,218

1951 81,46 3,173

1955 81,45 3,169

2003 81,45 3,179

In units of 10-4 16O/16

Ewald applied the expression below to derive the mass of 13C from 12CH. The massesof the reference isotopes are taken from the fractional packing curve f.

The values since 1951 arederived from a combinationof mass doublets and reactiondata.

Phys.Rev. 82 (1951) 756

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Mass measurements for 40A(r)

16O/16 12C/12 Year

39,971 39,958 1934/5

39,9754 39,9627 1937

39,97504 39,96234 1937

39,97555 39,96285 1940

39,9755 39,9628 1942

39,97551 39,96281 1949

39,97505 39,96235 1955

39,9750886 39,9623838 1960/2

39,9623842 1964

39,9623831 1977

39,9623837 1985

39,962383124 1993

39,962383130 1995/7

39,9623831225 2003

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What is wrong with the measurements with mass spectrometers?

Last minute addendum:

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Post-war activities - An early form of NUBASE?

The Kaiser-Wilhelm-Institut für Chemie had issued yearly progress reports on massessince around 1934. After the war, J. Mattauch compiled a small booklet in honour of Hahn’s 70th birthday. It comprised not only data on masses, but ,e.g., decay properties as half-lives. Seaborg had made available war-time data by sending the “Table of Isotopes” prior to publication.

In the following decades, mass evaluations normally contained only masses.

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The more recent history of nuclidic masses can be found in:

Georges Audi“The history of nuclidic masses and of their evaluation”International Journal of Mass Spectrometry 251 (2006) 85–94

55 years of modern mass evaluations (I)

An early (perhaps the first) attempt for a mass evaluation is M.S. Livingston, H.A. Bethe, “Nuclear Physics, C. Nuclear dynamics, experimental”Rev. Mod. Phys. 9 (1937) 245 XVIII. Nuclear masses; p. 366The authors combined data from mass spectrometry and nuclear reaction and decay data up to 40Ar.

In the early 1950’s it was found that the many relations (direct and indirect) between nuclides overdetermined the mass value of many nuclides.Aaldert H. Wapstra established a procedure using a least-squares method to solve the problem of overdetermination.The first table of atomic masses using this method is dated 1955.

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A.H. Wapstra, Physica 21 (1955) 367 + 385; J.R. Huizenga, Physica 21 (1955) 410F. Everling, L.A. König, J.H.E. Mattauch, A.H. Wapstra, Nucl. Phys. 18 (1960) 529L.A. König, J.H.E. Mattauch, A.H. Wapstra, Nucl. Phys. 31 (1962) 18R.R. Ries, R.A. Damerow, W.H. Johnson, Jr., Phys. Rev. 132 (1963) 1662 + 1673J.H.E. Mattauch, W. Thiele, A.H. Wapstra, Nucl. Phys. A67 (1965) 1 + 32 + 73

After the retirement of Mattauch in 1965, all AMEs (as far as I know) were directed by Aaldert H. Wapstra. A.H. Wapstra & K. Bos, At. Data Nucl. Data Tables 19 (1977) 175A.H. Wapstra, G. Audi & R. Hoekstra, Nucl. Phys. A432 (1985) 185G. Audi & A.H. Wapstra, Nucl. Phys. A 565 (1993) 66C. Borcea, G. Audi, A.H. Wapstra & P. Favaron, Nucl. Phys. A 565 (1993) 158G. Audi, A.H. Wapstra & M. Dedieu, Nucl. Phys. A 565 (1993) 193G. Audi & A.H. Wapstra, Nucl. Phys. A 595 (1995) 409G. Audi, O. Bersillon, J. Blachot & A.H. Wapstra, Nucl. Phys. A 624 (1997) 1G. Audi, O. Bersillon, J. Blachot & A.H. Wapstra, Nucl. Phys. A 729 (2003) 3A.H. Wapstra, G. Audi & C. Thibault, Nucl. Phys. A 729 (2003) 129G. Audi, A.H. Wapstra & C. Thibault, Nucl. Phys. A 729 (2003) 337

The Future AME (2013 ?) is prepared on a broader, international basis including Orsay, GSI, ANL, the Institute for Modern Physics, Lhanzou.

55 years of modern mass evaluations (II)

J. Mattauch

A.H. Wapstra

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R.R. Ries et al., “Atomic Masses from Ga to Mo”, Phys. Rev. 132 (1963) 1662R.A. Damerow et al.:”Atomic Masses from Ru to Xe”, Phys. Rev. 132 (1963) 1673

Local evaluations done in Minneapolis

Backbone of evaluation:Mass doublets measured with double-focusing mass spectrometers

Nuclear reaction and β-decaydata are then combined withthe masses of stable isotopesfrom the mass spectrometers.

Some mass doublet values fromthese papers are still listed in the 2003 Mass Evaluation!

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Progress in mass measurements and evaluations

AME 1955

AME 1977 AME 2003

A=120

?

1u = 16O/16

1u = 12C/12

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Atomic Mass Evaluation & NuBASE

AME 2003November 18, 2003

3504 masses3179 - ground-state masses 2228 experimental 951 estimations325 - isomers 201 experimental 122 estimations

Based on 7773 data, 374 not accepted:6169 valid input data4373 after compression by pre-averaging887 added from systematic trends

“Primary” data:• 1381 data representing 967 reactions and decays• 414 mass spectrometric data

From the 2228 experimental masseshave uncertainties• 192 < 1 keV• 1020 < 10 kev• 231 < 100 keV • 785 > 100 keV

This sample represents about half of the expected nuclides between the drip-lines.

Backbone from least-square calculation:System of 1381 equations for 847parameters (“primary” masses)

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AME2003 2009

(approximate values)

Masses 3504 3555

Data points (total) 7773 13080

Mass-doublets 4390

Mass-triplets 220

Reaction data 8470

Not used 374 7130‡

After preaveraging 4373 4760

Mass adjustment

“Primaries” equ. / unknowns

1381 / 847 1570 / 988

“secondaries 2770 2800

systematics 890 850

Progress in AME

‡ The new precise values (as, e.g., from trap measurements) in general supersede older ones.

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Long-range and multiple connections

Connections of input data for AME2003

133Cs

The mass evaluations up till nowcontain mostly connections between 2 (or a few) close lying neighbours.The future AMEs will in addition becharacterised by long-range relationsand complex connectivities betweenmultiple isotopes:• In the traps, nuclides are typically compared to easily ionisable refe- rence masses as 133Cs. The isotope 229Rn is 96 mass units distant from the reference mass.• Direct mass measurements by TOF in storage rings as ESR at GSI observe many nuclides simultane- ously. The masses are derived from correlation matrices which may con- tain up to 100.000 relations. This plenty of information is not (yet) taken into account in the actual AME.

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Future precision mass measurements

SHIPTRAP at GSI TRIGATRAP for reactor in Mainz

The project to build a mass spectrograph with a resolving power of 100.000 failed atthe MPI. Nowadays even higher precision measurements can be performed with Penning traps. One such instrument is connected to the velocity filter SHIP (which wasbuilt with the participation of Prof. Ewald). The work which once started at Berlinis now continued by the scientific off-spring.

And also at the Mainz TRIGA reactor (which is a legacy of Fritz Strassmann) a Penningtrap will continue the study of fission products.

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48Seminar für Kern- und Kosmochemie (“K&K Seminar”)MPI für Chemie, Mainz, Mittwoch, 10.2.2010, 17:15

Atomic Mass EvaluationsContributions of the Kaiser-Wilhelm-/Max-Planck-

Institut für Chemie

• For a long time, the KWI / MPI had been at the forefront of work dedicated to the study of radioactivity.• Also from the early days on, radioactive (and stable) isotopes have been applied in other fields as geology.• And there had always been a fruitful collaboration between scientists from neighbouring fields (as the very long interchange between the chemist Otto Hahn and the physicist Lise Meitner).• The work on atomic masses shifted in the course of the 1930‘s from chemistry to physics, but there remained close ties between the groups.• Influenced by my personal scientific background (as a „grandson“ of Ewald), I have presented in this seminar talk mainly work performed with mass spectrographs. • My actual work with the Atomic Mass Evaluation can be regarded as a return to the roots layed by Mattauch / Ewald in Dahlem, Tailfingen, Mainz, München.