Development of an Ultra-High Performance Multi-Turn TOF-SIMS/SNMS System “MULTUM-SIMS/SNMS”

  • Shingo EbataEmail author
  • Morio Ishihara
  • Kousuke Kumondai
  • Ryo Mibuka
  • Kiichiro Uchino
  • Hisayoshi Yurimoto
Research Article


A new system incorporating a multi-turn time-of-flight secondary ion/sputtered neutral mass spectrometer (TOF-SIMS/SNMS) with laser post-ionization was designed and constructed. This system consists of a gallium focused ion beam, femtosecond (fs) laser for post-ionization, and multi-turn TOF mass spectrometer. When laser post-ionization was used, the secondary ion signal strengths for several metals increased by up to 650 times, and were greater than the values obtained in conventional TOF-SIMS experiments. Use of the multi-turn mass spectrometer resulted in an increase in mass resolving power with increase in the total TOF. The mass resolving power reached to 23,000 after 800 multi-turn cycles, corresponding to a flight path length of 1040 m. These results indicated that this system is very effective for the analysis of valuable materials such as space samples with high sensitivity, high mass resolving power, and high lateral resolution.

Key words

Sputtered neutral mass spectrometry Time-of-flight mass spectrometer Gallium focused ion beam femtosecond (fs) laser post-ionization Space samples 



The authors acknowledge support for this study by a Grant-in-Aid for Creative Scientific Research (no. 16GS0214) provided by the Ministry of Education, Culture, Sports, Science, and Technology (MEXT), and was supported by the JSPS 141 Committee.

Supplementary material

13361_2012_528_MOESM1_ESM.jpg (1.2 mb)
Figure S1 (a) Photograph of the back of the novel TOF-SIMS system. There is laser injection window in the center of a sample chamber. (b) Photograph of laser optics and fs laser Integra-C. This photograph is the rearview of the one in Fig. 1. The fs laser beam was ejected from the Integra-C output window and injected into the sample chamber through laser optics consisting of mirrors and a lens (JPEG 1244 kb)
13361_2012_528_MOESM2_ESM.jpg (110 kb)
Figure S2 Schematic of the laser optics and the interior of the sample chamber. The laser optics system consisted of three mirrors and one lens. The fs laser was focused on the area at a distance of ~100 μm from the sample surface, and terminated by a Al2O3-SUS plate (JPEG 110 kb)
13361_2012_528_MOESM3_ESM.jpg (673 kb)
Figure S3 Schematic of MULTUM II. The linear and multi-turn mode was conducted by turning on/off the sector I and IV (JPEG 672 kb)
13361_2012_528_MOESM4_ESM.jpg (330 kb)
Figure S4 Au+ signals (a) without laser irradiation and (b) with laser irradiation. Au+ signals were significantly enhanced (by up to 650 times) when the fs laser was combined with SIMS. In addition, Au2 + signals were also detected with laser irradiation (JPEG 330 kb)
13361_2012_528_MOESM5_ESM.jpg (267 kb)
Figure S5 Intensity ratio plots of SNMS mode/SIMS mode showing variation of the signal intensity rations of the twelve measured elements (C, Mg, Al, Si, Ti, Fe, Cu, Pd, Ag, Pt, Au, and Pb). For all elements, signal intensities were increased by laser post-ionization (JPEG 267 kb)
13361_2012_528_MOESM6_ESM.jpg (411 kb)
Figure S6 Evaluation of mass resolving power using the developed system. (a) In linear mode, and (b) in multi-turn mode. In the linear mode, m/∆m was calculated to be 500, while in the multimode it was calculated to be 7500. The mass resolving power improved with increasing numbers of cycles (JPEG 410 kb)
13361_2012_528_MOESM7_ESM.jpg (235 kb)
Figure S7 Relationship between mass resolving power of Al+ signal and multi-turn cycle number of MULTUM-SIMS/SNMS. The mass resolving power increased with increasing multi-turn cycles. Flight path length of single multi-turn cycle corresponds to 1.3 m (JPEG 235 kb)
13361_2012_528_MOESM8_ESM.jpg (468 kb)
Figure S8 Calculated chemical compositions of JB-2. Black circles indicate the SNMS. White squares indicate the SIMS mode. The RSF of the gray area ranged from 1 to 10. This suggests that the post-ionization method can improve the sensitivities as well as measure the chemical compositions (JPEG 467 kb)


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Copyright information

© American Society for Mass Spectrometry 2013

Authors and Affiliations

  • Shingo Ebata
    • 1
    • 4
    Email author
  • Morio Ishihara
    • 1
  • Kousuke Kumondai
    • 1
  • Ryo Mibuka
    • 2
  • Kiichiro Uchino
    • 2
  • Hisayoshi Yurimoto
    • 3
    • 4
  1. 1.Department of PhysicsOsaka UniversityToyonakaJapan
  2. 2.Graduate School of Engineering SciencesKyushu UniversityKasugaJapan
  3. 3.Department of Natural History SciencesHokkaido UniversitySapporoJapan
  4. 4.Isotope Imaging Laboratory, CRISHokkaido UniversitySapporoJapan

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