Evidence of impurities in thiolated single-stranded DNA oligomers and their effect on DNA self-assembly on gold

Citation

Lee, C. Y.; Canavan, H. E.; Gamble, L. J.; & Castner, D. G. (2005). Evidence of impurities in thiolated single-stranded DNA oligomers and their effect on DNA self-assembly on gold. Langmuir, 21(11), 5134-5141.

Abstract

The diversity of techniques used in the synthesis, treatment, and purification of the single-stranded DNA oligomers containing a thiol anchor group (SH-ssDNA) has led to a significant variation in the purity of commercially available SH-ssDNA. In this work, we use X-ray photoelectron spectroscopy (XPS) and time-of-flight secondary ion mass spectrometry (ToF-SIMS) to study how the impurities present in commercially synthesized SH-ssDNA oligomers affected the structure of the resulting DNA films on Au. XPS results indicate that two of the purchased SH-ssDNA oligomers contain excess carbon and sulfur. The molecular fragmentation patterns obtained with ToF-SIMS were used to determine the identity of several contaminants in the DNA films, including poly(dimethylsiloxane) (PDMS), lipid molecules, and sulfur-containing molecules. In particular, the ToF-SIMS results determined that the excess sulfur detected by XPS was due to the presence of dithiothreitol, a reductant often used to cleave disulfide precursors. Furthermore, we found that the SH-ssDNA self-assembly process is affected by the presence of these contaminants. When relatively pure SH-ssDNA is used to prepare the DNA films, the P, N, O, and C atomic percentages were observed by XPS to increase over a 24-h time period. In contrast, surfaces prepared using SH-ssDNA containing higher levels of contaminants did not follow this trend. XPS result indicates that, after the initial SH-ssDNA adsorption, the remaining material incorporated into these films was due to contamination.

Keyword(s)

covalent attachment
dip-pen nanolithography
hybridization
immobilization
monolayer films
nanostructures
oligonucleotides
ray photoelectron-spectroscopy
surface-plasmon resonance
tris(2-carboxyethyl)phosphine

Notes

928AP
Times Cited:30
Cited References Count:43

Reference Type

Journal Article

Secondary Title

Langmuir

Author(s)

Lee, C. Y.
Canavan, H. E.
Gamble, L. J.
Castner, D. G.

Year Published

2005

Date Published

1748044800

Volume Number

21

Issue Number

11

Pages

5134-5141

DOI

Doi 10.1021/La0472302