Polynucleotide adsorption to negatively charged surfaces in divalent salt solutions.

Polynucleotide adsorption to negatively charged surfaces via divalent ions is extensively used in the study of biological systems. We analyze here the adsorption mechanism via a self-consistent mean-field model that includes the pH effect on the surface-charge density and the interactions between divalent ions and surface groups. The adsorption is driven by the cooperative effect of divalent metal ion condensation along polynucleotides and their reaction with the surface groups. Although the apparent reaction constants are enhanced by the presence of polynucleotides, the difference between reaction constants of different divalent ions at the ideal condition explains why not all divalent cations mediate DNA adsorption onto anionic surfaces. Calculated divalent salt concentration and pH value variations on polynucleotide adsorption are consistent with atomic force microscope results. Here we use long-period x-ray standing waves to study the adsorption of mercurated-polyuridylic acid in a ZnCl2 aqueous solution onto a negatively charged hydroxyl-terminated silica surface. These in situ x-ray measurements, which simultaneously reveal the Hg and Zn distribution profiles along the surface normal direction, are in good agreement with our model. The model also provides the effects of polyelectrolyte line-charge density and monovalent salt on adsorption.

[1]  M. Bedzyk,et al.  Direct observation of cations and polynucleotides explains polyion adsorption to like-charged surfaces. , 2005, The journal of physical chemistry. B.

[2]  Richard W. Gurney,et al.  Comparative X-ray standing wave analysis of metal-phosphonate multilayer films of dodecane and porphyrin molecular square. , 2005, The journal of physical chemistry. B.

[3]  R. Netz.  Water and ions at interfaces , 2004 .

[4]  M. Muthukumar,et al.  Theory of counter-ion condensation on flexible polyelectrolytes: adsorption mechanism. , 2004, The Journal of chemical physics.

[5]  Hao-Bin Cheng,et al.  Adsorption of rod-like polyelectrolytes onto weakly charged surfaces , 2003 .

[6]  Stéphane Fusil,et al.  Adsorption of DNA to mica mediated by divalent counterions: a theoretical and experimental study. , 2003, Biophysical journal.

[7]  A. Dobrynin,et al.  Effect of Short-Range Interactions on Polyelectrolyte Adsorption at Charged Surfaces† , 2003 .

[8]  Rhiju Das,et al.  Counterion distribution around DNA probed by solution X-ray scattering. , 2003, Physical review letters.

[9]  P. González-Mozuelos,et al.  Association in electrolyte solutions: Rodlike polyelectrolytes in multivalent salts , 2003 .

[10]  F. Solis.  Phase diagram of dilute polyelectrolytes: Collapse and redissolution by association of counterions and co-ions , 2002, cond-mat/0204591.

[11]  K. Kremer,et al.  Like-charge colloid-polyelectrolyte complexation , 2002, cond-mat/0201515.

[12]  K. Kremer,et al.  Conformation of a polyelectrolyte complexed to a like-charged colloid. , 2001, Physical review. E, Statistical, nonlinear, and soft matter physics.

[13]  I. Szleifer,et al.  Kinetics and thermodynamics of protein adsorption: a generalized molecular theoretical approach. , 2001, Biophysical journal.

[14]  C. Safinya,et al.  DNA condensation in two dimensions. , 2000, Proceedings of the National Academy of Sciences of the United States of America.

[15]  Sens,et al.  Counterion release and electrostatic adsorption , 2000, Physical review letters.

[16]  J. Joanny,et al.  Adsorption of semiflexible polyelectrolytes on charged planar surfaces: Charge compensation, charge reversal, and multilayer formation. , 1999 .

[17]  C. Bustamante,et al.  Facilitated Target Location on DNA by IndividualEscherichia coli RNA Polymerase Molecules Observed with the Scanning Force Microscope Operating in Liquid* , 1999, The Journal of Biological Chemistry.

[18]  W. Gelbart,et al.  Spontaneous overcharging of macro-ion complexes , 1999 .

[19]  B. D. de Grooth,et al.  Direct visualization of dynamic protein-DNA interactions with a dedicated atomic force microscope. , 1998, Biophysical journal.

[20]  M. Lieber,et al.  Interaction of DNA‐dependent protein kinase with DNA and with Ku: biochemical and atomic‐force microscopy studies , 1997, The EMBO journal.

[21]  P K Hansma,et al.  Escherichia coli RNA polymerase activity observed using atomic force microscopy. , 1997, Biochemistry.

[22]  P. Hansma,et al.  Reversible Binding of DNA to Mica for AFM Imaging , 1996 .

[23]  T. Thundat,et al.  Direct atomic force microscope imaging of EcoRI endonuclease site specifically bound to plasmid DNA molecules. , 1996, Proceedings of the National Academy of Sciences of the United States of America.

[24]  V. Bloomfield,et al.  Macroion Attraction Due to Electrostatic Correlation between Screening Counterions. 1. Mobile Surface-Adsorbed Ions and Diffuse Ion Cloud , 1996 .

[25]  H. Hansma,et al.  DNA binding to mica correlates with cationic radius: assay by atomic force microscopy. , 1996, Biophysical journal.

[26]  M. L. Garg,et al.  K and L Shell X-Ray Fluorescence Cross Sections , 1995 .

[27]  M. O. D. L. Cruz,et al.  Ion condensation in salt‐free dilute polyelectrolyte solutions , 1995 .

[28]  S. Marčelja,et al.  Charge reversal seen in electrical double layer interaction of surfaces immersed in 2:1 calcium electrolyte , 1993 .

[29]  Y. Lyubchenko,et al.  Atomic force microscopy of long DNA: imaging in air and under water. , 1993, Proceedings of the National Academy of Sciences of the United States of America.

[30]  C. Siegerist,et al.  Reproducible Imaging and Dissection of Plasmid DNA Under Liquid with the Atomic Force Microscope , 1992, Science.

[31]  G. M. Bommarito,et al.  Diffuse-double layer at a membrane-aqueous interface measured with x-ray standing waves. , 1990, Science.

[32]  G. M. Bommarito,et al.  X-ray standing waves: a molecular yardstick for biological membranes. , 1988, Science.

[33]  L. T. Zhuravlev.  Concentration of hydroxyl groups on the surface of amorphous silicas , 1987 .

[34]  R. Iler.  The Chemistry of Silica: Solubility, Polymerization, Colloid and Surface Properties and Biochemistry of Silica , 1979 .

[35]  G. S. Manning.  Limiting laws and counterion condensation in polyelectrolyte solutions. IV. The approach to the limit and the extraordinary stability of the charge fraction. , 1977, Biophysical chemistry.

[36]  D. C. Livingston,et al.  Direct covalent mercuration of nucleotides and polynucleotides. , 1975, Biochemistry.

[37]  R. M. Izatt,et al.  Sites and thermodynamic quantities associated with proton and metal ion interaction with ribonucleic acid, deoxyribonucleic acid, and their constituent bases, nucleosides, and nucleotides. , 1971, Chemical reviews.

[38]  Gerald S. Manning,et al.  Limiting Laws and Counterion Condensation in Polyelectrolyte Solutions I. Colligative Properties , 1969 .

[39]  L. G. Parratt.  Surface Studies of Solids by Total Reflection of X-Rays , 1954 .

[40]  R. Netz,et al.  Poisson-Boltzmann theory for membranes with mobile charged lipids and the pH-dependent interaction of a DNA molecule with a membrane. , 2002, Biophysical journal.

[41]  H. Hansma.  Surface biology of DNA by atomic force microscopy. , 2001, Annual review of physical chemistry.

[42]  C. Bustamante,et al.  Visualizing protein-nucleic acid interactions on a large scale with the scanning force microscope. , 1996, Annual review of biophysics and biomolecular structure.

[43]  D. E. Yates,et al.  Site-binding model of the electrical double layer at the oxide/water interface , 1974 .

[44]  S. Lowen.  The Biophysical Journal , 1960, Nature.