Details
| Original language | English |
|---|---|
| Pages (from-to) | 3257-3273 |
| Number of pages | 17 |
| Journal | ANALYST |
| Volume | 148 |
| Issue number | 14 |
| Publication status | Published - 21 Jun 2023 |
| Externally published | Yes |
Abstract
Ion mobility spectrometry (IMS), which can be employed as either a stand-alone instrument or coupled to mass spectrometry, has become an important tool for analytical chemistry. Because of the direct relation between an ion's mobility and its structure, which is intrinsically related to its collision cross section (CCS), IMS techniques can be used in tandem with computational tools to elucidate ion geometric structure. Here, we present MobCal-MPI 2.0, a software package that demonstrates excellent accuracy (RMSE 2.16%) and efficiency in calculating low-field CCSs via the trajectory method (≤30 minutes on 8 cores for ions with ≤70 atoms). MobCal-MPI 2.0 expands on its predecessor by enabling the calculation of high-field mobilities through the implementation of the 2nd order approximation to two-temperature theory (2TT). By further introducing an empirical correction to account for deviations between 2TT and experiment, MobCal-MPI 2.0 can compute accurate high-field mobilities that exhibit a mean deviation of <4% from experimentally measured values. Moreover, the velocities used to sample ion-neutral collisions were updated from a weighted to a linear grid, enabling the near-instantaneous evaluation of mobility/CCS at any effective temperature from a single set of N2 scattering trajectories. Several enhancements made to the code are also discussed, including updates to the statistical analysis of collision event sampling and benchmarking of overall performance.
ASJC Scopus subject areas
- Chemistry(all)
- Analytical Chemistry
- Biochemistry, Genetics and Molecular Biology(all)
- Biochemistry
- Environmental Science(all)
- Environmental Chemistry
- Chemistry(all)
- Spectroscopy
- Chemistry(all)
- Electrochemistry
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In: ANALYST, Vol. 148, No. 14, 21.06.2023, p. 3257-3273.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - MobCal-MPI 2.0
T2 - an accurate and parallelized package for calculating field-dependent collision cross sections and ion mobilities
AU - Haack, Alexander
AU - Ieritano, Christian
AU - Hopkins, W. Scott
N1 - Funding Information: The authors would like to thank Dr Jeff Crouse for his help during the early stages of this work. Further, the authors would like to acknowledge the high-performance computing support from the Digital Research Alliance of Canada. W. S. H. would like to acknowledge the financial support provided by the Natural Sciences and Engineering Research Council (NSERC) of Canada in the form of Discovery and Alliance grants. Further, W. S. H. acknowledges the support from the InnoHK Initiative and the Hong Kong Special Administrative Region Government. A. H. gratefully acknowledges this work being funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) – 449651261. C. I. acknowledges financial support from the Government of Canada for the Vanier Canada Graduate Scholarship.
PY - 2023/6/21
Y1 - 2023/6/21
N2 - Ion mobility spectrometry (IMS), which can be employed as either a stand-alone instrument or coupled to mass spectrometry, has become an important tool for analytical chemistry. Because of the direct relation between an ion's mobility and its structure, which is intrinsically related to its collision cross section (CCS), IMS techniques can be used in tandem with computational tools to elucidate ion geometric structure. Here, we present MobCal-MPI 2.0, a software package that demonstrates excellent accuracy (RMSE 2.16%) and efficiency in calculating low-field CCSs via the trajectory method (≤30 minutes on 8 cores for ions with ≤70 atoms). MobCal-MPI 2.0 expands on its predecessor by enabling the calculation of high-field mobilities through the implementation of the 2nd order approximation to two-temperature theory (2TT). By further introducing an empirical correction to account for deviations between 2TT and experiment, MobCal-MPI 2.0 can compute accurate high-field mobilities that exhibit a mean deviation of <4% from experimentally measured values. Moreover, the velocities used to sample ion-neutral collisions were updated from a weighted to a linear grid, enabling the near-instantaneous evaluation of mobility/CCS at any effective temperature from a single set of N2 scattering trajectories. Several enhancements made to the code are also discussed, including updates to the statistical analysis of collision event sampling and benchmarking of overall performance.
AB - Ion mobility spectrometry (IMS), which can be employed as either a stand-alone instrument or coupled to mass spectrometry, has become an important tool for analytical chemistry. Because of the direct relation between an ion's mobility and its structure, which is intrinsically related to its collision cross section (CCS), IMS techniques can be used in tandem with computational tools to elucidate ion geometric structure. Here, we present MobCal-MPI 2.0, a software package that demonstrates excellent accuracy (RMSE 2.16%) and efficiency in calculating low-field CCSs via the trajectory method (≤30 minutes on 8 cores for ions with ≤70 atoms). MobCal-MPI 2.0 expands on its predecessor by enabling the calculation of high-field mobilities through the implementation of the 2nd order approximation to two-temperature theory (2TT). By further introducing an empirical correction to account for deviations between 2TT and experiment, MobCal-MPI 2.0 can compute accurate high-field mobilities that exhibit a mean deviation of <4% from experimentally measured values. Moreover, the velocities used to sample ion-neutral collisions were updated from a weighted to a linear grid, enabling the near-instantaneous evaluation of mobility/CCS at any effective temperature from a single set of N2 scattering trajectories. Several enhancements made to the code are also discussed, including updates to the statistical analysis of collision event sampling and benchmarking of overall performance.
UR - http://www.scopus.com/inward/record.url?scp=85164276781&partnerID=8YFLogxK
U2 - 10.1039/d3an00545c
DO - 10.1039/d3an00545c
M3 - Article
C2 - 37376881
AN - SCOPUS:85164276781
VL - 148
SP - 3257
EP - 3273
JO - ANALYST
JF - ANALYST
SN - 0003-2654
IS - 14
ER -