Title: CHILI – the Chicago Instrument for Laser Ionization – a new tool for isotope measurements in cosmochemistry

Abstract

Here, we describe CHILI, the Chicago Instrument for Laser Ionization, a new resonance ionization mass spectrometer developed for isotopic analysis at high spatial resolution and high sensitivity of small samples like contemporary interstellar dust grains returned by the Stardust spacecraft. We explain how CHILI addresses the technical challenges associated with such analyses by pushing most technical specifications towards their physical limits. As an initial demonstration, after many years of designing and developing CHILI, we have analyzed presolar silicon carbide grains for their isotopic compositions of strontium, zirconium, and barium. Subsequently, after further technical improvements, we have used CHILI to analyze, for the first time without interference, all stable isotopes of iron and nickel simultaneously in presolar silicon carbide grains. With a special timing scheme for the ionization lasers, we separated iron and nickel isotopes in the time-of-flight spectrum such that the isobaric interference between ⁵⁸Fe and ⁵⁸Ni was resolved. In-depth discussion of the astrophysical implications of the presolar grain results is deferred to dedicated later publications. Here we focus on the technical aspects of CHILI, its status quo, and further developments necessary to achieve CHILI’s ultimate goals, 10 nm lateral resolution and 30–40% useful yield.

Authors:

Stephan, Thomas  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-6377-8731"

Trappitsch, Reto  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-0924-236X"

Davis, Andrew M.  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-7955-6236"

Pellin, Michael J.  ^[2];

• Search DOE PAGES for author "Pellin, Michael J."
• Search DOE PAGES for ORCID "0000-0002-8149-9768"

Rost, Detlef ^[3]; Savina, Michael R. ^[4]; Yokochi, Reika ^[1]; Liu, Nan  ^[5]

• Search DOE PAGES for author "Liu, Nan"
• Search DOE PAGES for ORCID "0000-0002-4811-8679"

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+ Show Author Affiliations

1. The Univ. of Chicago, Chicago, IL (United States); Chicago Center for Cosmochemistry, Chicago, IL (United States)
2. The Univ. of Chicago, Chicago, IL (United States); Chicago Center for Cosmochemistry, Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
3. The Univ. of Chicago, Chicago, IL (United States); Chicago Center for Cosmochemistry, Chicago, IL (United States); Univ. of Auckland, Auckland (New Zealand)
4. Chicago Center for Cosmochemistry, Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
5. The Univ. of Chicago, Chicago, IL (United States); Chicago Center for Cosmochemistry, Chicago, IL (United States); Carnegie Institution for Science, Washington, D.C. (United States)

Publication Date:

Fri Jun 17 00:00:00 EDT 2016

Research Org.:

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Org.:

USDOE

OSTI Identifier:

1329356

Report Number(s):

LLNL-JRNL-688285
Journal ID: ISSN 1387-3806

Grant/Contract Number:  

AC52-07NA27344

Resource Type:

Accepted Manuscript

Journal Name:

International Journal of Mass Spectrometry

Additional Journal Information:

Journal Volume: 407; Journal Issue: C; Journal ID: ISSN 1387-3806

Publisher:

Elsevier

Country of Publication:

United States

Language:

English

Subject:

42 ENGINEERING; 79 ASTRONOMY AND ASTROPHYSICS; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; resonance ionization mass spectrometry; cosmochemistry; isotopes; isobaric interference