Abstract
RECENT developments have made electrospray-ionization (ESI) mass spectrometry1–3 an important technique for measuring molecular weights and studying the structures of large molecules of relative molecular masses approaching 200,000 (Mr 200K). Analysis of still larger molecules is difficult, however: to obtain a mass/charge ratio within the detectable limits, the ions must bear several charges, but a collection of ions of differing multiple charges presents a spectrum that is hard to interpret. This problem would be avoided if sufficient sensitivity can be achieved to detect individual molecules. Here we describe a technique that realizes this sensitivity for molecules of Mr to ~7 x 106, and which has the potential to be extended to Mr≈109. We use ESI and Fouriertransform ion cyclotron resonance mass spectrometry4 to obtain repeated measurements of the mass-to-charge ratio of single, highly charged molecular ions. We are able to observe stepwise changes in the charge of an isolated ion owing to its reaction with small molecules introduced into the detection cell. This technique should have wide applications for characterization of polymers and large biomolecules.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 51 print issues and online access
$199.00 per year
only $3.90 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Meng, C. K., Mann, M. & Fenn, J. B. Z. Phys. D10, 361–368 (1988).
Fenn, J. B., Mann, M., Meng, C. K., Wong, S. F. & Whitehouse, C. M. Science 246, 64–71 (1989).
Smith, R. D., Loo, J. A., Edmonds, C. G., Barinaga, C. J. & Udseth, H. R. Analyt. Chem. 62, 882–899 (1990).
Marshall, A. G. Accts Chem. Res. 18, 316–322 (1985).
Nohmi, T. & Fenn, J. B. J. Am. chem. Soc. 114, 3241–3246 (1992).
Xu, Y., Bae, R. J., Beuhler, R. J. & Friedman, L. J. phys. Chem. 97, 11883–11886 (1993).
Henry, K. D., Quinn, J. P. & McLafferty, F. W. J. Am. chem. Soc. 113, 5447–5449 (1991).
Marshall, A. G. & Grosshans, P. B. Analyt. Chem. 63, A215–A229 (1991).
Williams, E. R., Henry, K. D., McLafferty, F. W., Shabanowitz, J. & Hunt, D. F. J. Am. chem. Soc. 12, 6157–6162 (1990).
Winger, B. E., Hofstadler, S. A., Bruce, J. E., Udseth, H. R. & Smith, R. D. J. Am. Soc. Mass Spectrom. 4, 566–577 (1993).
Limbach, P. A., Grosshans, P. B. & Marshall, A. G. Analyt. Chem. 65, 135–140 (1993).
Bruce, J. E. et al. J. Am. chem. Soc. (submitted).
Smith, R. D. & Light-Wahl, K. J. Biol. Mass Spectrom. 22, 493–501 (1993).
Author information
Authors and Affiliations
Rights and permissions
About this article
Cite this article
Smith, R., Cheng, X., Brace, J. et al. Trapping, detection and reaction of very large single molecular ions by mass spectrometry. Nature 369, 137–139 (1994). https://doi.org/10.1038/369137a0
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1038/369137a0
This article is cited by
-
Ultralong transients enhance sensitivity and resolution in Orbitrap-based single-ion mass spectrometry
Nature Methods (2024)
-
Mass spectrometry using electrospray ionization
Nature Reviews Methods Primers (2023)
-
Frequency chasing of individual megadalton ions in an Orbitrap analyser improves precision of analysis in single-molecule mass spectrometry
Nature Chemistry (2022)
-
The emerging landscape of single-molecule protein sequencing technologies
Nature Methods (2021)
-
Enhanced Multiplexing in Fourier Transform Charge Detection Mass Spectrometry by Decoupling Ion Frequency from Mass to Charge Ratio
Journal of the American Society for Mass Spectrometry (2019)
Comments
By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.
