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@PHDTHESIS{Bergmann:354739,
      author       = {Bergmann, Julian},
      title        = {{H}igh-{R}esolution {T}andem {M}ass {S}pectrometry of
                      complex mixtures with a {M}ultiple-{R}eflection
                      {T}ime-of-{F}light {M}ass-{S}pectrometer},
      school       = {Justus Liebig University Giessen},
      type         = {Dissertation},
      publisher    = {Universitätsbibliothek Gießen},
      reportid     = {GSI-2024-01213},
      pages        = {119},
      year         = {2024},
      note         = {Dissertation, Justus Liebig University Giessen, 2024},
      abstract     = {In this work, a multiple-reflection time-of-flight mass
                      spectrometer (MR-TOF-MS) was adapted and employed, for the
                      first time, for ultra-high resolution analytical tandem mass
                      spectrometry. The device was deployed to analyze isobaric
                      molecules in a heavy crude oil sample and to derive new
                      structure formulas thanks to the device's ultra-high
                      separation power and advanced data analysis techniques. A
                      new atmospheric pressure interface (API) was built to
                      operate multiple ion sources in parallel and to optimize the
                      transmission for viscous samples, like crude oil residue. A
                      radio-frequency carpet funnels the ions to the RFQ transport
                      line, providing a compact, efficient, and fast method to
                      combine ions from different sources in parallel to introduce
                      calibrants, while avoiding chemical reactions with the
                      analyte. Ion sources of three different types, nano-ESI,
                      micro-ESI, and thermal 133Cs, were designed, built, coupled
                      to the API, and operated to acquire the data shown in this
                      thesis. A software package was developed for operating the
                      device and for acquiring and analyzing mass spectra. The
                      software allows automatically setting up the measurement by
                      converting parameters like the desired mass range to
                      voltages and HV pulse sequences in real time. Further
                      automated measurement features are a time-of-flight drift
                      correction, a scanning of measurement parameters, and an
                      automatic gain control. In addition, its calibration
                      technique and its enhanced elemental composition
                      identification further assist in analysis. Furthermore, data
                      analysis procedures were developed to increase the mass
                      range, while retaining a high mass accuracy and mass
                      resolving power for closed-path MR-TOF-MS. The software is
                      also used together with MR-TOF-MS devices at particle
                      accelerators, i.e. the MR-TOF-MS of the FRS Ion Catcher at
                      GSI, Darmstadt, and the MR-TOF-MS of the TITAN experiment at
                      TRIUMF in Vancouver. The device in this work features a mass
                      resolving power (FWHM) of up to 300000, a sensitivity down
                      to 10 mol/l, a linear dynamic range of five orders of
                      magnitude, and mass accuracy of 0.3 ppm. Its re-trapping
                      technique allows for a precursor mass separation power of up
                      to 250000 at an efficiency of 10 $\%$ or up to 100000 with
                      an efficiency of 80 $\%$ for tandem mass spectrometry. These
                      capabilities were shown for tandem mass spectrometry
                      measurements up to the fourth stage $(MS^4).$ Furthermore,
                      molecules as heavy as human insulin (5810 u) have been
                      analyzed. Tandem mass spectrometry of a sample of
                      medium-heavy crude oil residue was performed and four
                      isobaric mass signals close to 322.2 u/e were isolated with
                      an isolation window of 10 mu and a suppression factor of
                      200. This was only possible thanks to this device's
                      ultra-high mass separation power. The resulting fragments
                      within a mass range of 300 - 500 u were measured at a mass
                      resolving power of 200000 and a mass accuracy of better than
                      1 ppm, and their elemental compositions were identified.
                      With the help of our collaboration with the workgroup Mass
                      Spectrometry of Prof. Dr. Wolfgang Schrader at the Max
                      Planck Institute für Kohleforschung in Mülheim an der
                      Ruhr, 26 molecular structures for the two isobaric precursor
                      molecules, C23H32N+ and C23H28ON+, were identified. For
                      future applications of the device, investigation of less
                      understood crude oil samples as well as applications in life
                      sciences are envisioned.},
      keywords     = {Massenspektrometrie (Other) / analytische
                      Massenspektrometrie (Other) / MR-TOF-MS (Other) /
                      Multiple-reflection time-of-flight mass spectrometers
                      (Other) / crude oil (Other) / Rohöl (Other) / Ionenoptik
                      (Other) / Software (Other) / Gerätesteuerung (Other) /
                      Datenanalyse (Other) / Geräteentwicklung (Other) /
                      Simulationen (Other) / Experiment (Other) / Tandem
                      Massenspektrometrie (Other) / Massenselektiver Wiedereinfang
                      (Other) / Mass-selective re-trapping (Other) / IONAS (Other)
                      / Scheidenberger (Other) / ddc:530 (Other)},
      cin          = {FRS / SuperFRS-EC@FAIR},
      cid          = {I:(DE-Ds200)FRS-20110310OR124 /
                      I:(DE-Ds200)Coll-FAIR-SuperFRS-EC},
      pnm          = {612 - Cosmic Matter in the Laboratory (POF4-612)},
      pid          = {G:(DE-HGF)POF4-612},
      experiment   = {$EXP:(DE-Ds200)Experiment_without_proposal_number-20200803$},
      typ          = {PUB:(DE-HGF)11},
      doi          = {10.22029/JLUPUB-18381},
      url          = {https://repository.gsi.de/record/354739},
}