Mixed DNA/oligo (ethylene glycol) functionalized gold surfaces improve DNA hybridization in complex media
Biointerphases volume 1, pages 82–92 (2006)
Reliable, direct “sample-to-answer” capture of nucleic acid targets from complex media would greatly improve existing capabilities of DNA microarrays and biosensors. This goal has proven elusive for many current nucleic acid detection technologies attempting to produce assay results directly from complex real-world samples, including food, tissue, and environmental materials. In this study, we have investigated mixed self-assembled thiolated single-strand DNA (ssDNA) monolayers containing a short thiolated oligo (ethylene glycol) (OEG) surface diluent on gold surfaces to improve the specific capture of DNA targets from complex media. Both surface composition and orientation of these mixed DNA monolayers were characterized with x-ray photoelectron spectroscopy (XPS) and near-edge x-ray absorption fine structure (NEXAFS). XPS results from sequentially adsorbed ssDNA/OEG monolayers on gold indicate that thiolated OEG diluent molecules first incorporate into the thiolated ssDNA monolayer and, upon longer OEG exposures, competitively displace adsorbed ssDNA molecules from the gold surface. NEXAFS polarization dependence results #followed by monitoring the N 1s → π* transition) indicate that adsorbed thiolated ssDNA nucleotide base-ring structures in the mixed ssDNA monolayers are oriented more parallel to the gold surface compared to DNA bases in pure ssDNA monolayers. This supports ssDNA oligomer reorientation towards a more upright position upon OEG mixed adlayer incorporation. DNA target hybridization on mixed ssDNA probe/OEG monolayers was monitored by surface plasmon resonance (SPR). Improvements in specific target capture for these ssDNA probe surfaces due to incorporation of the OEG diluent were demonstrated using two model biosensing assays, DNA target capture from complete bovine serum and from salmon genomic DNA mixtures. SPR results demonstrate that OEG incorporation into the ssDNA adlayer improves surface resistance to both nonspecific DNA and protein adsorption, facilitating detection of small DNA target sequences from these undiluted, unpurified complex biological mixtures unachievable with previously reported, analogous ssDNA/11-mercapto-1-undecanol monolayer surfaces [P. Gong, C.-Y. Lee, L. J. Gamble, D. G. Castner, and D.W. Grainger, Anal. Chem. 78, 3326 (2006)].
S. Hahn, S. Mergenthaler, B. Zimmermann, and W. Holzgreve, Bioelectrochemistry 67, 151 (2005).
P. A. E. Piunno and U. J. Krull, Anal. Bioanal. Chem. 381, 1004 (2005).
P. Gong, C.-Y. Lee, L. J. Gamble, D. G. Castner, and D. W. Grainger, Anal. Chem. 78, 3326 (2006).
C.-Y. Lee, P. Gong, G. M. Harbers, D. W. Grainger, D. G. Castner, and L. J. Gamble, Anal. Chem. 78, 3316 (2006).
M. Lochhead, C. A. Greef, P. Gong, and D. W. Grainger, in Microarrays: Methods and Protocols (Methods in Molecular Biology), 2nd ed. (Humana Press, Totowa, NJ, in press).
R. Georgiadis, K. P. Peterlinz, and A. W. Peterson, J. Am. Chem. Soc. 122, 3166 (2000).
A. W. Peterson, R. J. Heaton, and R. Georgiadis, J. Am. Chem. Soc. 122, 7837 (2000).
A. W. Peterson, R. J. Heaton, and R. M. Georgiadis, Nucleic Acids Res. 29, 5163 (2001).
A. W. Peterson, L. K. Wolf, and R. M. Georgiadis, J. Am. Chem. Soc. 124, 14601 (2002).
B. P. Nelson, T. E. Grimsrud, M. R. Liles, R. M. Goodman, and R. M. Corn, Anal. Chem. 73, 1 (2001).
Y. K. Cho, S. Kim, Y. A. Kim, H. K. Lim, K. Lee, D. S. Yoon, G. Lim, Y. E. Pak, T. H. Ha, and K. Kim, J. Colloid Interface Sci. 278, 44 (2004).
F. Caruso, E. Rodda, D. N. Furlong, and V. Haring, Sens. Actuators B 41, 189 (1997).
R. Levicky, T. M. Herne, M. J. Tarlov, and S. K. Satija, J. Am. Chem. Soc. 120, 9787 (1998).
T. M. Herne and M. J. Tarlov, J. Am. Chem. Soc. 119, 8916 (1997).
H. J. Lee, Y. Li, A. W. Wark, and R. M. Corn, Anal. Chem. 77, 5096 (2005).
T. T. Goodrich, H. J. Lee, and R. M. Corn, J. Am. Chem. Soc. 126, 4086 (2004).
L. K. Ista, H. Y. Fan, O. Baca, and G. P. Lopez, FEMS Microbiol. Lett. 142, 59 (1996).
K. L. Prime and G. M. Whitesides, J. Am. Chem. Soc. 115, 10714 (1993).
K. Bergstrom, K. Holmberg, A. Safranj, A. S. Hoffman, M. J. Edgell, A. Kozlowski, B. A. Hovanes, and J. M. Harris, J. Biomed. Mater. Res. 26, 779 (1992).
C. Palegrosdemange, E. S. Simon, K. L. Prime, and G. M. Whitesides, J. Am. Chem. Soc. 113, 12 (1991).
C. Boozer, J. Ladd, S. F. Chen, Q. Yu, J. Homola, and S. Y. Jiang, Anal. Chem. 76, 6967 (2004).
C. Y. Lee, H. E. Canavan, L. J. Gamble, and D. G. Castner, Langmuir 21, 5134 (2005).
K. E. Nelson, L. Gamble, L. S. Jung, M. S. Boeckl, E. Naeemi, S. L. Golledge, T. Sasaki, D. G. Castner, C. T. Campbell, and P. S. Stayton, Langmuir 17, 2807 (2001).
J. L. Lenhart, R. L. Jones, E. K. Lin, C. L. Soles, W. L. Wu, D. A. Fischer, S. Sambasivan, D. L. Goldfarb, and M. Angelopoulos, J. Vac. Sci. Technol. B 20, 2920 (2002).
J. Stohr, NEXAFS Spectroscopy (Springer, New York, 1992).
L. S. Jung, C. T. Campbell, T. M. Chinowsky, M. N. Mar, and S. S. Yee, Langmuir 14, 5636 (1998).
P. G. Wu, B. S. Fujimoto, L. Song, and J. M. Schurr, Biophys. Chem. 41, 217 (1991).
R. E. Harrington, J. Am. Chem. Soc. 92, 6957 (1970).
J. E. Darnell and H. Lodish, Molecular Cell Biology (Scientific American, New York, 1990).
J. Mandel, The Statistical Analysis of Experimental Data (Dover, New York, 1984).
C. J. May, H. E. Canavan, and D. G. Castner, Anal. Chem. 76, 1114 (2004).
G. Beamson and D. Briggs, High Resolution XPS of Organic Polymers (Wiley, West Sussex, 1992).
D. G. Castner, K. Hinds, and D. W. Grainger, Langmuir 12, 5083 (1996).
N. T. Samuel, C.-Y. L. Lee, L. J. Gamble, D. A. Fisher, and D. G. Castner, J. Electron Spectrosc. Relat. Phenom. 152, 134 (2006).
D. Y. Petrovykh, V. Perez-Dieste, A. Opdahl, H. Kimura-Suda, J. M. Sullivan, M. J. Tarlov, F. J. Himpsel, and L. J. Whitman, J. Am. Chem. Soc. 128, 2 (2006).
J. N. Crain, A. Kirakosian, J. L. Lin, Y. D. Gu, R. R. Shah, N. L. Abbott, and F. J. Himpsel, J. Appl. Phys. 90, 3291 (2001).
A. G. Shard, J. D. Whittle, A. J. Beck, P. N. Brookes, N. A. Bullett, R. A. Talib, A. Mistry, D. Barton, and S. L. McArthur, J. Phys. Chem. B 108, 12472 (2004).
M. Zwahlen, D. Brovelli, W. Caseri, and G. Hahner, J. Colloid Interface Sci. 256, 262 (2002).
M. Zharnikov, Y. Ouchi, M. Hasegawa, and A. Scholl, J. Phys. Chem. B 108, 859 (2004).
M. G. Samant, J. Stohr, H. R. Brown, T. P. Russell, J. M. Sands, and S. K. Kumar, Macromolecules 29, 8334 (1996).
G. Hahner, M. Kinzler, C. Thummler, C. Woll, and M. Grunze, J. Vac. Sci. Technol. A 10, 2758 (1992).
D. A. Outka, J. Stohr, J. P. Rabe, and J. D. Swalen, J. Chem. Phys. 88, 4076 (1988).
N. L. Anderson and N. G. Anderson, Mol. Cell Proteomics 1, 845 (2002).
N. L. Rosi and C. A. Mirkin, Chem. Rev. (Washington, D.C.) 105, 1547 (2005).
About this article
Cite this article
Lee, CY., Gamble, L.J., Grainger, D.W. et al. Mixed DNA/oligo (ethylene glycol) functionalized gold surfaces improve DNA hybridization in complex media. Biointerphases 1, 82–92 (2006). https://doi.org/10.1116/1.2219110