v r LA-12522-C Conference Proceedings of the Alfred O. Nier Symposium on Inorganic Mass Spectrometry May 7-9, 1991 Durango, Colorado DISTRfaUTION OF TH« DOCUMENT MB Sponsored by the US Department of Energy (Office of Basic Energy Sciences/Geosciences) and the Los Alamos National Laboratory's Isotope and Nuclear Chemistry Group J Los Alamos National Laboratory is operated by the University of California for the United States Department of Energy undercontrac! W-7405-BNG-36. An Affirmative Action/Equal Opportunity Employer This report.was prepared as an account of work sponsored by an agency of the United States Government. Neither The Regents of the University of California, the United States Government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apftaratus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or sen'ice by trade name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by The Regents of the Unwersity of California, the United States Government, or any agency thereof. The viezes and opinions of authors expressed herein do not necessarily slate or reflect those of Vie Regents of the Unwersity of California, the United States Government, or any agency thereof. LA-12522-C Conference UC-401 and UC-410 Issued: May 1993 Proceedings of the Alfred O. Nier Symposium on Inorganic Mass Spectrometry Durango, Colorado May 7-9,1991 Compiled and Edited by Donald J. Rokop DlSTRfaUTlON OF TH» DOCUMENT 16 UNU Los Alamos NATIONAL LABORATORY Los Alamos, New Mexico 87545 Acknowledgements A. O. Nier Symposium Publications Design and Word Processing Elaine Roybal Technical Reviewers B. L. Fearey M. T. Murrell C. T. Olinger H. Poths D. J. Rokop B. M. Tissue Editing Jody H. Hieken Design Consultant G. L. Tietjen A. O. Nier Symposium Coordination Suzie Salazar Christy Archuleta Elaine Roybal A. O. Nier Symposium Logo W. G. Zaelke CONTENTS Welcome vii Dedication viii Introduction 1 Papers 3 Speaker Abstracts 217 Poster Abstracts 231 Symposium Schedule 253 Index of Presenters 257 At the initial session of the Alfred O. Nier Symposium on Inorganic Mass Spectrometry, Alexander Gancarz, Isotope and Nuclear Chemistry Division Leader, welcomed the participants. It is a real honor for the Isotope and Nuclear Chemistry Division of the Los Alamos National Laboratory to be cosponsoring this meeting with the Department of Energy Office of Basic Energy Sciences, Division of Engineering and Geosciences. I am pleased to welcome you to this meeting, The Alfred O. Nier Symposium on Inorganic Mass Spectrometry, which celebrates the 80th birthday of A. O. Nier. The response from the scientific community has been truly overwhelming, including not only his colleagues and former students, but also many enthused professionals from the fields of geochemistry and mass spectrometry that Al was so instrumental in founding. The great variety in the talks to be presented in the next three days is most exciting and reflects the viability of inorganic mass spectrometry. There are clearly many opportunities for instrumental advances—particularly for increased abundance sensitivity on smaller and smaller samples as well as enhanced trace analysis capabilities. What is also remarkable is the wide range of scientific endeavors in which mass spectrometry is crucial. One of the talks contains the concept of "from the Heavens and the Deep Earth," and many of the presentations at this symposium reflect this remarkably wide spectra. We will hear discussions on subjects ranging from samples and processes deep within the earth, to environmental information deduced from isotopes, on ozone in the earth's atmosphere, on extraterrestrial samples, and finally—outwards to Stardust and isotopic astronomy. It is also exciting to see the use of inorganic mass spectrometry in the life sciences, including human metabolism and nutrition. I again want to issue a warm welcome and look forward to lively discussions with each of you over the next three days. Alexander J. Gancarz Division Leader Isotope and Nuclear Chemistry Division VII Dedication It is our privilege to honor one of the outstanding scientists of the past 50 years, Professor Alfred O. C. Nier. His career began as an undergraduate at the University of Minnesota almost 65 years ag' .nd continues today as Regents Professor of Physics Emeritus. His productivity and expertise in the practical application of fundamental principles for measuring the abundances of isotopes and the interpretation of these measurements is unequalled. I, myself, am a third generation "Nier," having been trained by one of his early students, Charlie Stevens, formerly of Argonne National Laboratory. There are many generations of unsuspecting 'Nier' descendants around us today, some of whom have never ever considered building a mass spectrometer! I suspect that the serendipitous juxtaposition of Al Nier, the then modern vacuum technology, and the development of the electrometer In 1940, Professor Nier is at the console of the first 60° sector mass tube in the late 1930s and early spectrometer. (Note the acid bums in his iab coat.) 1940s has directly resulted in this week's gathering. This Minnesota in 1945 that or to speculate on all the juxtaposition has undoubtedly Professor Nier began the work implications and further strongly contributed to the that spawned our careers. His developments resulting from development of modern isotope landmark publication, his early experiments. I do geology, geochronology, and frequently referred to only as know that two of his early atomic and nuclear physics. "RSI 1947," described for the efforts contributed to a whole first time an operational, new world: the demonstration Although he did a great practical mass spectrometer that that B5U was the isotope deal of the initial development was available to any researcher responsible for slow neutron work at the University of with the means to build one. fission and the development of Minnesota during the early There is no way to the technology to purify it. 1930s and at Harvard in the late adequately describe Professor I recently perused Professor 1930s, it was after he returned to Nier's many accomplishments Nier's Curriculum Vitae and viii Dedication came across this statement, "Research Interests: Development of mass spectrometers and application to problems in nuclear physics, chemistry, biology, engineering, geology and geophysics." Like the man himself— concise, straight forward, and to the point. Over the years, his scientific work has crossed many lines of discipline and touched a multitude of different communities. What kind of curiosity motivates a man to apply his particular expertise to such a wide variety of problems? Despite pioneering in so many areas, how can he Professor Nier and Harold Washburn (VP Research) at the console of have achieved such a Nier's 60° mass spectrometer, whose design he had given to Consolidated phenomenal success rate? (Pasadena, 1948). He is indeed a rare combination of man and scientist and teacher. It is in this last role, teacher, that he has probably made his most valuable contribution to us all. For we all—all of us here this week—have sat in his classroom and benefited from the perceptive knowledge of Professor Alfred O. C. Nier. Donald J. Rokop Isotope Geochemistry Los Alamos National Laboratory At the Gulf Oil Research In 1966, Dr. Nier is appointed Laboratory in Pittsburgh, Dr. Nier Regents Professor of Physics. presents a lecture (1955). IX ALFRED O. NIER SYMPOSIUM ON INORGANIC MASS SPECTROMETRY Edited by D. J. Rokop ABSTRACT In May 1991, over 100 inorganic mass spectroscopists, including representatives from 9 different countries, gathered in Durango, Colorado, to discuss cross-discipline research. The cross fertilization generated from this meeting prompted a spontaneous and universal request to repeat the experience. This proceedings contains summaries of papers and poster sessions presented at this symposium and gives some feel for our motivation in planning future meetings of this nature. INTRODUCTION Gatherings of mass spectroscopists throughout the world have, for some years, been dominated by organic application specialists. Inorganic specialists have found themselves being diluted out of the system. When one attended a professional meeting, one had to look very hard to find someone of similar interests. With the deemphasis on nuclear energy in this country, the decreased involvement in the weapons program, and the shift of inorganic mass spectroscopists to the geological arena, almost any meeting featuring mass spectrometry is dominated by organic applications. For some years I have been thinking that it would be appropriate to have a meeting of inorganic applications specialists featuring the wide variety of applications in the inorganic arena, without any organic types present. I tossed this idea around with many of you and subsequently abandoned it when I considered all the work involved. How could it be successful? What theme could it possibly use to draw all these diverse specialists together? The answer was right on my doorstep. We were awaiting the arrival of a very famous and well-liked man to consult at our Laboratory, Professor Alfred O. Nier. Introduction When I contacted Professor Nier to ask his permission to organize this event, he not only agreed with the idea, but agreed with the whole premise for doing it. He pointed out to me that it hadn't been done like this since the early 1950s, by Hippie at the National Bureau of Standards. I am sort of a third generation Nier, having been initially trained at Argonne National Laboratory by Charley Stevens, one of Nier's early students. While I was talking to Professor Nier, the subject of his long history in the field came up along with the fact that the meeting would almost coincide with his 80th birthday.