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      Imaging Mass Spectrometry on the Nanoscale with Cluster Ion Beams

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      Publication date (Electronic):
      Journal: Analytical Chemistry
      Publisher: American Chemical Society

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          Abstract

          Imaging with cluster secondary ion mass spectrometry (SIMS) is reaching a mature level of development. Using a variety of molecular ion projectiles to stimulate desorption, 3-dimensional imaging with the selectivity of mass spectrometry can now be achieved with submicrometer spatial resolution and <10 nm depth resolution. In this Perspective, stock is taken regarding what it will require to routinely achieve these remarkable properties. Issues include the chemical nature of the projectile, topography formation, differential erosion rates, and perhaps most importantly, ionization efficiency. Shortcomings of existing instrumentation are also noted. Speculation about how to successfully resolve these issues is a key part of the discussion.

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          Improvement of biological time-of-flight-secondary ion mass spectrometry imaging with a bismuth cluster ion source.

          David Touboul, Felix Kollmer, Ewald Niehuis … (2005)
          A new liquid metal ion gun (LMIG) filled with bismuth has been fitted to a time-of-flight-secondary ion mass spectrometer (TOF-SIMS). This source provides beams of Bi(n)q+ clusters with n = 1-7 and q = 1 and 2. The appropriate clusters have much better intensities and efficiencies than the Au3+ gold clusters recently used in TOF-SIMS imaging, and allow better lateral and mass resolution. The different beams delivered by this ion source have been tested for biological imaging of rat brain sections. The results show a great improvement of the imaging capabilities in terms of accessible mass range and useful lateral resolution. Secondary ion yields Y, disappearance cross sections sigma, efficiencies E = Y/sigma , and useful lateral resolutions deltaL have been compared using the different bismuth clusters, directly onto the surface of rat brain sections and for several positive and negative secondary ions with m/z ranging from 23 up to more than 750. The efficiency and the imaging capabilities of the different primary ions are compared by taking into account the primary ion current for reasonable acquisition times. The two best primary ions are Bi3+ and Bi5(2+). The Bi3+ ion beam has a current at least five times larger than Au3+ and therefore is an excellent beam for large-area imaging. Bi5(2+) ions exhibit large secondary ions yields and a reasonable intensity making them suitable for small-area images with an excellent sensitivity and a possible useful lateral resolution <400 nm.
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            A C60 primary ion beam system for time of flight secondary ion mass spectrometry: its development and secondary ion yield characteristics.

            Daniel Weibel, Steve Wong, Nicholas P. Lockyer … (2003)
            A buckminsterfullerene (C60)-based primary ion beam system has been developed for routine application in TOF-SIMS analysis of organic materials. The ion beam system is described, and its performance is characterized. Nanoamp beam currents of C60+ are obtainable in continuous current mode. C60(2+) can be obtained in pulsed mode. At 10 keV, the beam can be focused to less than 3 microm with 0.1 nA currents. TOF-SIMS studies of a series of molecular solids and a number of polymer systems in monolayer and thick film forms are reported. Very significant enhancement of secondary ion yields, particularly at higher mass, were observed using 10-keV C60+ for all samples other than PTFE, as compared to those observed from 10 keV Ga+ primary ions. Three materials (PS2000, Irganox 1010, PET) were studied in detail to investigate primary ion-induced disappearance (damage) cross sections to determine the increase in secondary ion formation efficiency. The C60 disappearance cross sections observed from monolayer film PS2000 and self-supporting PET film are close to those observed from Ga+. The resulting C60 efficiencies are 30-100 times those observed from gallium. The cross sections observed from C60 bombardment of multilayer molecular solids are approximately 100 times less, such that essentially zero damage sputtering is possible. The resulting efficiencies are > 10(3) greater than from gallium. It is also shown that C60 primary ions do not generate any more low-mass fragments than any other ion beam system does. C60 is shown to be a very favorable ion beam system for TOF-SIMS, delivering high yield, close to 10% total yield, favoring high-mass ions, and on thick samples, offering the possibility of analysis well beyond the static limit.
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              TOF-SIMS 3D imaging of native and non-native species within HeLa cells.

              Jeremy Brison, Michael A Robinson, Danielle Benoit … (2013)
              In this study, a non-native chemical species, bromodeoxyuridine (BrdU), was imaged within single HeLa cells using time-of-flight secondary ion mass spectrometry (TOF-SIMS). z-corrected 3D images were reconstructed that accurately portray the distribution of intracellular BrdU as well as other intracellular structures. The BrdU was localized to the nucleus of cells, whereas structures composed of CxHyOz(-) species were located in bundles on the periphery of cells. The CxHyOz(-) subcellular features had a spatial resolution at or slightly below a micrometer (900 nm), as defined by the distance between the 16% and 84% intensities in a line scan across the edge of the features. Additionally, important parameters influencing the quality of the HeLa cell 3D images were investigated. Atomic force microscopy measurements revealed that the HeLa cells were sputtered at a rate of approximately 4 nm per 10(13) C60(+) ions/cm(2) at 10 keV and a 45° incident angle. Optimal 3D images were acquired using a Bi3(+) liquid metal ion gun operating in the simultaneous high mass and spatial resolution mode.
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                Author and article information

                Journal
                Journal ID (nlm-ta): Anal Chem
                Journal ID (iso-abbrev): Anal. Chem
                Journal ID (publisher-id): ac
                Journal ID (coden): ancham
                Title: Analytical Chemistry
                Publisher: American Chemical Society
                ISSN (Print): 0003-2700
                ISSN (Electronic): 1520-6882
                Publication date PMC-release: 02 December 2015
                Publication date (Electronic): 02 December 2014
                Publication date (Print): 06 January 2015
                Volume: 87
                Issue: 1
                Pages: 328-333
                Affiliations
                [1]Department of Chemistry, Penn State University , University Park, Pennsylvania 16875, United States
                Author notes
                [* ]E-mail: nxw@ 123456psu.edu .
                Article
                DOI: 10.1021/ac503650p
                PMC ID: 4287836
                PubMed ID: 25458665
                SO-VID: 719da41c-eded-4a25-8eaa-3c53db0f2315
                Copyright © Copyright © 2014 American Chemical Society
                License:

                This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.

                History
                Date received : 29 September 2014
                Date accepted : 02 December 2014
                Funding
                National Institutes of Health, United States
                Categories
                Subject: Perspective
                Custom metadata
                document-id-old-9 ac503650p
                document-id-new-14 ac-2014-03650p
                ccc-price

                ScienceOpen disciplines: Analytical chemistry
                Data availability:
                ScienceOpen disciplines: Analytical chemistry

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