Role of Alumina Coatings for Selective and Controlled Bonding of DNA on Technologically Relevant Oxide Surfaces

DNA immobilization on surfaces is crucial to a number of applications. However, detailed understanding of DNA/surface chemistry remains poorly documented, especially on oxide surfaces, due to the complexity of such large molecules. This work focuses on a simpler molecule, 2-deoxythymidine-5-monophosphate (dTMP), which contains all the chemical elements of DNA. It confirms that adsorption of dTMP onto OH-terminated SiO2 surfaces does not result in a chemical bond (dTMP readily washes off) and instead shows that dTMP chemically adsorbs on Al2O3 surfaces. We combine first-principles calculations, X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared (FTIR) spectroscopy to determine the bonding configuration of dTMP onto alumina surfaces controllably grown by atomic layer deposition. We demonstrate that dTMP covalently reacts with alumina. Calculations indicate that covalent bonding of all dTMP polar groups (sugar ring, phosphate group, and thymine) is thermodynamically favored. Spectroscopic ...

[1]  Paul W K Rothemund,et al.  Optimized assembly and covalent coupling of single-molecule DNA origami nanoarrays. , 2014, ACS nano.

[2]  K. Yager,et al.  A general strategy for the DNA-mediated self-assembly of functional nanoparticles into heterogeneous systems. , 2013, Nature nanotechnology.

[3]  C. Morari,et al.  Effect of van der Waals interaction on the geometric and electronic properties of DNA nucleosides adsorbed on Cu(111) surface: a DFT study. , 2013, The journal of physical chemistry. A.

[4]  Weihong Tan,et al.  Self-assembled, aptamer-tethered DNA nanotrains for targeted transport of molecular drugs in cancer theranostics , 2013, Proceedings of the National Academy of Sciences.

[5]  Jun-Hyung Cho,et al.  Physisorption of DNA nucleobases on h -BN and graphene: VdW-corrected DFT calculations , 2013, 1302.7171.

[6]  Nicholas M. Fahrenkopf,et al.  Immobilization mechanisms of deoxyribonucleic acid (DNA) to hafnium dioxide (HfO2) surfaces for biosensing applications. , 2012, ACS applied materials & interfaces.

[7]  Y. Chabal,et al.  Activation of surface hydroxyl groups by modification of H-terminated Si(111) surfaces. , 2012, Journal of the American Chemical Society.

[8]  Carole Rossi,et al.  High‐Energy Al/CuO Nanocomposites Obtained by DNA‐Directed Assembly , 2012 .

[9]  Grigory Tikhomirov,et al.  DNA-based programming of quantum dot valency, self-assembly and luminescence. , 2011, Nature nanotechnology.

[10]  Faisal A. Aldaye,et al.  Organization of Intracellular Reactions with Rationally Designed RNA Assemblies , 2011, Science.

[11]  Jan E Schnitzer,et al.  Overcoming in vivo barriers to targeted nanodelivery. , 2011, Wiley interdisciplinary reviews. Nanomedicine and nanobiotechnology.

[12]  Clive R. Bagshaw,et al.  Site-Specific Assembly of DNA-Based Photonic Wires by Using Programmable Polyamides , 2011, Angewandte Chemie.

[13]  Hao Yan,et al.  Encapsulation of gold nanoparticles in a DNA origami cage. , 2011, Angewandte Chemie.

[14]  P. Tinnefeld,et al.  Single-molecule four-color FRET visualizes energy-transfer paths on DNA origami. , 2011, Journal of the American Chemical Society.

[15]  A. Turberfield,et al.  DNA-templated protein arrays for single-molecule imaging. , 2011, Nano letters.

[16]  Kersten S. Rabe,et al.  Orthogonal protein decoration of DNA origami. , 2010, Angewandte Chemie.

[17]  Robert M. Dirks,et al.  Selective cell death mediated by small conditional RNAs , 2010, Proceedings of the National Academy of Sciences.

[18]  K. Sarveswaran,et al.  Guided deposition of individual DNA nanostructures on silicon substrates. , 2010, Langmuir : the ACS journal of surfaces and colloids.

[19]  Hao Yan,et al.  Immobilization and one-dimensional arrangement of virus capsids with nanoscale precision using DNA origami. , 2010, Nano letters.

[20]  M. Halls,et al.  Surface and interface processes during atomic layer deposition of copper on silicon oxide. , 2010, Langmuir : the ACS journal of surfaces and colloids.

[21]  Hua Yang,et al.  Metal-nucleic acid cages. , 2009, Nature chemistry.

[22]  T. Caykara,et al.  DNA immobilization on polymer-modified Si surface by controlling pH , 2009 .

[23]  W. Schneider,et al.  DFT Investigation of Intermediate Steps in the Hydrolysis of α-Al2O3(0001) , 2009 .

[24]  D. Lelie,et al.  DNA-guided crystallization of colloidal nanoparticles , 2008, Nature.

[25]  Russell P. Goodman,et al.  A self-assembled DNA bipyramid. , 2007, Journal of the American Chemical Society.

[26]  E. M. Fernández,et al.  Ab initio calculations of H2O and O2 adsorption on Al2O3 substrates , 2007 .

[27]  Bong Jin Hong,et al.  DNA-DNA interaction on dendron-functionalized sol-gel silica films followed with surface plasmon fluorescence spectroscopy. , 2007, Journal of colloid and interface science.

[28]  P. Rothemund Folding DNA to create nanoscale shapes and patterns , 2006, Nature.

[29]  S. Grimme Semiempirical hybrid density functional with perturbative second-order correlation. , 2006, The Journal of chemical physics.

[30]  F. Weigend,et al.  Balanced basis sets of split valence, triple zeta valence and quadruple zeta valence quality for H to Rn: Design and assessment of accuracy. , 2005, Physical chemistry chemical physics : PCCP.

[31]  Andrew J Turberfield,et al.  The single-step synthesis of a DNA tetrahedron. , 2004, Chemical communications.

[32]  Marek Sierka,et al.  Fast evaluation of the Coulomb potential for electron densities using multipole accelerated resolution of identity approximation , 2003 .

[33]  M. Tarlov,et al.  Quantitative analysis and characterization of DNA immobilized on gold. , 2003, Journal of the American Chemical Society.

[34]  N. Seeman DNA in a material world , 2003, Nature.

[35]  Lloyd M. Smith,et al.  DNA Attachment and Hybridization at the Silicon (100) Surface , 2002 .

[36]  Lloyd M. Smith,et al.  Covalent attachment of oligodeoxyribonucleotides to amine-modified Si (001) surfaces. , 2000, Nucleic acids research.

[37]  Lloyd M. Smith,et al.  Synthesis and Characterization of DNA-Modified Silicon (111) Surfaces , 2000 .

[38]  G. Rivas,et al.  Electrochemically Induced Release of DNA from Gold Ultramicroelectrodes , 1999 .

[39]  D. Pang,et al.  DNA-modified electrodes - Part 3: spectroscopic characterization of DNA-modified gold electrodes , 1999 .

[40]  G. Kresse,et al.  From ultrasoft pseudopotentials to the projector augmented-wave method , 1999 .

[41]  R. Nichols,et al.  In-situ infrared spectroscopic studies of thymine adsorption on a Au(111) electrode , 1998 .

[42]  T. M. Herne,et al.  Characterization of DNA Probes Immobilized on Gold Surfaces , 1997 .

[43]  Burke,et al.  Generalized Gradient Approximation Made Simple. , 1996, Physical review letters.

[44]  Kresse,et al.  Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. , 1996, Physical review. B, Condensed matter.

[45]  J. Storhoff,et al.  A DNA-based method for rationally assembling nanoparticles into macroscopic materials , 1996, Nature.

[46]  A. Ulman,et al.  Formation and Structure of Self-Assembled Monolayers. , 1996, Chemical reviews.

[47]  Marco Häser,et al.  Auxiliary basis sets to approximate Coulomb potentials (Chem. Phys. Letters 240 (1995) 283-290) , 1995 .

[48]  Marco Häser,et al.  Auxiliary basis sets to approximate Coulomb potentials , 1995 .

[49]  P. Blöchl Projector augmented-wave method. , 1994, Physical review. B, Condensed matter.

[50]  Hans W. Horn,et al.  ELECTRONIC STRUCTURE CALCULATIONS ON WORKSTATION COMPUTERS: THE PROGRAM SYSTEM TURBOMOLE , 1989 .

[51]  J. Koenig,et al.  F.t.-i.r. and laser-Raman spectra of thymine and thymidine , 1984 .

[52]  A. Hughes,et al.  A comparison of weak molecular adsorption of organic molecules on clean copper and platinum surfaces , 1984 .

[53]  Erik Winfree,et al.  Self-assembly of carbon nanotubes into two-dimensional geometries using DNA origami templates. , 2010, Nature nanotechnology.

[54]  L. Blum,et al.  DNA biosensors and microarrays. , 2008, Chemical reviews.

[55]  R. Nichols,et al.  Adsorption of Thymine on Gold Single-Crystal Electrodes , 1997 .

[56]  A. Klamt,et al.  COSMO : a new approach to dielectric screening in solvents with explicit expressions for the screening energy and its gradient , 1993 .

[57]  W. R. Wadt,et al.  Ab initio effective core potentials for molecular calculations. Potentials for main group elements Na to Bi , 1985 .

[58]  D. Clark,et al.  Molecular core binding energies; carbon and nitrogen 1s levels for cytosine and thymine , 1970 .