Electrospray-Ionization Mass Spectrometry for Screening the Specificity and Stability of Single-Stranded-DNA Templated Self-Assemblies
✍ Scribed by Pim G. A. Janssen; Joost L. J. van Dongen; E. W. Meijer; Albertus P. H. J. Schenning
- Publisher
- John Wiley and Sons
- Year
- 2008
- Tongue
- English
- Weight
- 478 KB
- Volume
- 15
- Category
- Article
- ISSN
- 0947-6539
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✦ Synopsis
Abstract
Supramolecular complexes consisting of a single‐stranded oligothymine (dT__n__) as the host template and an array of guest molecules equipped with a complementary diaminotriazine hydrogen‐bonding unit have been studied with electrospray‐ionization mass spectrometry (ESI‐MS). In this hybrid construct, a supramolecular stack of guest molecules is hydrogen bonded to dT__n__. By changing the hydrogen‐bonding motif of the DNA host template or the guest molecules, selective hydrogen bonding was proven. We were able to detect single‐stranded‐DNA (ssDNA)–guest complexes for strands with lengths of up to 20 bases, in which the highest complex mass detected was 15 kDa; these complexes constitute 20‐component self‐assembled objects. Gas‐phase breakdown experiments on single‐ and multiple‐guest–DNA assemblies gave qualitative information on the fragmentation pathways and the relative complex stabilities. We found that the guest molecules are removed from the template one by one in a highly controlled way. The stabilities of the complexes depend mainly on the molecular weight of the guest molecules, a fact suggesting that the complexes collapse in the gas phase. By mixing two different guests with the ssDNA template, a multicomponent dynamic library can be created. Our results demonstrate that ESI‐MS is a powerful tool to analyze supramolecular ssDNA complexes in great detail.