Details
| Original language | English |
|---|---|
| Pages (from-to) | 2711-2725 |
| Number of pages | 15 |
| Journal | Journal of the American Society for Mass Spectrometry |
| Volume | 30 |
| Issue number | 12 |
| Early online date | 21 Nov 2019 |
| Publication status | Published - 1 Dec 2019 |
| Externally published | Yes |
Abstract
The use of differential mobility spectrometry (DMS) as a separation tool prior to mass analysis has increased in popularity over the years. However, the fundamental principles behind the difference between high- and low-field mobility is still a matter of debate—especially regarding the strong impact of solvent molecules added to the gas phase in chemically modified DMS environments. In this contribution, we aim to present a thorough model for the determination of the ion mobility over a wide range of field strengths and subsequent calculation of DMS dispersion plots. Our model relies on first principle calculations only, incorporating the modeling of the “hard-sphere” mobility, the change in CCS with field strength, and the degree of clustering of solvent molecules to the ion. We show that all three factors have to be taken into account to qualitatively predict dispersion plots. In particular, type A behavior (i.e., strong clustering) in DMS can only be explained by a significant change of the mean cluster size with field strengths. The fact that our model correctly predicts trends between differently strong binding solvents, as well as the solvent concentration and the background gas temperature, highlights the importance of clustering for differential mobility. [Figure not available: see fulltext.].
Keywords
- Collision cross section, Dispersion plot, DMS, Ion mobility, Population distribution
ASJC Scopus subject areas
- Biochemistry, Genetics and Molecular Biology(all)
- Structural Biology
- Chemistry(all)
- Spectroscopy
Cite this
- Standard
- Harvard
- Apa
- Vancouver
- BibTeX
- RIS
In: Journal of the American Society for Mass Spectrometry, Vol. 30, No. 12, 01.12.2019, p. 2711-2725.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - A First Principle Model of Differential Ion Mobility
T2 - the Effect of Ion-Solvent Clustering
AU - Haack, Alexander
AU - Crouse, Jeff
AU - Schlüter, Femke Jutta
AU - Benter, Thorsten
AU - Hopkins, W. Scott
PY - 2019/12/1
Y1 - 2019/12/1
N2 - The use of differential mobility spectrometry (DMS) as a separation tool prior to mass analysis has increased in popularity over the years. However, the fundamental principles behind the difference between high- and low-field mobility is still a matter of debate—especially regarding the strong impact of solvent molecules added to the gas phase in chemically modified DMS environments. In this contribution, we aim to present a thorough model for the determination of the ion mobility over a wide range of field strengths and subsequent calculation of DMS dispersion plots. Our model relies on first principle calculations only, incorporating the modeling of the “hard-sphere” mobility, the change in CCS with field strength, and the degree of clustering of solvent molecules to the ion. We show that all three factors have to be taken into account to qualitatively predict dispersion plots. In particular, type A behavior (i.e., strong clustering) in DMS can only be explained by a significant change of the mean cluster size with field strengths. The fact that our model correctly predicts trends between differently strong binding solvents, as well as the solvent concentration and the background gas temperature, highlights the importance of clustering for differential mobility. [Figure not available: see fulltext.].
AB - The use of differential mobility spectrometry (DMS) as a separation tool prior to mass analysis has increased in popularity over the years. However, the fundamental principles behind the difference between high- and low-field mobility is still a matter of debate—especially regarding the strong impact of solvent molecules added to the gas phase in chemically modified DMS environments. In this contribution, we aim to present a thorough model for the determination of the ion mobility over a wide range of field strengths and subsequent calculation of DMS dispersion plots. Our model relies on first principle calculations only, incorporating the modeling of the “hard-sphere” mobility, the change in CCS with field strength, and the degree of clustering of solvent molecules to the ion. We show that all three factors have to be taken into account to qualitatively predict dispersion plots. In particular, type A behavior (i.e., strong clustering) in DMS can only be explained by a significant change of the mean cluster size with field strengths. The fact that our model correctly predicts trends between differently strong binding solvents, as well as the solvent concentration and the background gas temperature, highlights the importance of clustering for differential mobility. [Figure not available: see fulltext.].
KW - Collision cross section
KW - Dispersion plot
KW - DMS
KW - Ion mobility
KW - Population distribution
UR - http://www.scopus.com/inward/record.url?scp=85075337859&partnerID=8YFLogxK
U2 - 10.1007/s13361-019-02340-1
DO - 10.1007/s13361-019-02340-1
M3 - Article
C2 - 31755046
AN - SCOPUS:85075337859
VL - 30
SP - 2711
EP - 2725
JO - Journal of the American Society for Mass Spectrometry
JF - Journal of the American Society for Mass Spectrometry
SN - 1044-0305
IS - 12
ER -