Collapse of DNA under alternating electric fields.

Recent studies have shown that double-stranded DNA can collapse in the presence of a strong electric field. Here we provide an in-depth study of the collapse of DNA under weak confinement in microchannels as a function of buffer strength, driving frequency, applied electric-field strength, and molecule size. We find that the critical electric field at which DNA molecules collapse (tens of kV/m) is strongly dependent on driving frequency (100-800 Hz) and molecular size (20-160 kbp), and weakly dependent on the ionic strength (8-60 mM). We argue that an apparent stretching at very high electric fields is an artifact of the finite frame time of video microscopy.

[1]  B. Shklovskii WIGNER CRYSTAL MODEL OF COUNTERION INDUCED BUNDLE FORMATION OF RODLIKE POLYELECTROLYTES , 1998, cond-mat/9809429.

[2]  I. Rubinstein,et al.  POLARIZATION OF NON-EQUILIBRIUM DOUBLE LAYER AND AGGLOMERATION OF POLYELECTROLYTE BALLS , 2002 .

[3]  Cesare Cametti,et al.  Dielectric spectroscopy and conductivity of polyelectrolyte solutions , 2004 .

[4]  Won Kyu Kim,et al.  Charge density coordination and dynamics in a rodlike polyelectrolyte. , 2008, Physical review. E, Statistical, nonlinear, and soft matter physics.

[5]  Leonid Shtilman,et al.  Voltage against current curves of cation exchange membranes , 1979 .

[6]  R. Netz,et al.  Anomalous birefringence and polarizability saturation of charged elastic rods: Field-strength, salt and finite-concentration effects , 2008 .

[7]  Albert van den Berg,et al.  Concentration polarization in translocation of DNA through nanopores and nanochannels. , 2012, Physical review letters.

[8]  Roland G. Winkler,et al.  Polyelectrolyte electrophoresis: Field effects and hydrodynamic interactions , 2008 .

[9]  Y. Feldman,et al.  Dielectric relaxation measurements of 12 kbp plasmid DNA. , 2000, Biochimica et biophysica acta.

[10]  M. Fixman,et al.  Spherical macroions in strong fields , 1983 .

[11]  R. Bates,et al.  Conductance of tris(hydroxymethyl)-aminomethane hydrochloride (Tris·HCl) in water at 25 and 37°C , 1980 .

[12]  C. Cametti,et al.  Effect of ions on counterion fluctuation in low-molecular weight DNA dielectric dispersions. , 1984, Biophysical journal.

[13]  W. Helfrich,et al.  Deformation of spherical vesicles by electric fields , 1988 .

[14]  Murat Okandan,et al.  Combined field-induced dielectrophoresis and phase separation for manipulating particles in microfluidics , 2003 .

[15]  Eric Lee,et al.  Electrophoresis of a single charged porous sphere in an infinite medium of electrolyte solution. , 2013, Journal of colloid and interface science.

[16]  H. Isambert,et al.  Electrohydrodynamically induced aggregation during constant and pulsed field capillary electrophoresis of DNA. , 1999, Biopolymers.

[17]  G. S. Manning A field-dissociation relation for polyelectrolytes with an application to field-induced conformational changes of polynucleotides. , 1977, Biophysical chemistry.

[18]  M. Musheev,et al.  Stable DNA aggregation by removal of counterions. , 2013, Analytical chemistry.

[19]  H. Sinn,et al.  Counterions between charged polymers exhibit liquid-like organization and dynamics. , 2006, Proceedings of the National Academy of Sciences of the United States of America.

[20]  R. Larson,et al.  Stretching of a single tethered polymer in a uniform flow. , 1995, Science.

[21]  M. Eigen,et al.  Orientation field effect of polyelectrolytes in solution , 1957 .

[22]  D. Anselmetti,et al.  Molecular mechanisms and kinetics between DNA and DNA binding ligands. , 2005, Biophysical journal.

[23]  Sebastian Fischer,et al.  Low-frequency collective exchange mode in the dielectric spectrum of salt-free dilute polyelectrolyte solutions , 2013, The European Physical Journal E.

[24]  E. Furst,et al.  Anomalous particle rotation and resulting microstructure of colloids in AC electric fields. , 2008, Langmuir : the ACS journal of surfaces and colloids.

[25]  C. Wälti,et al.  Establishment of the ac electrokinetic elongation mechanism of DNA by three-dimensional fluorescent imaging , 2006 .

[26]  R. Seidel,et al.  Mechanical and structural properties of YOYO-1 complexed DNA , 2010, Nucleic acids research.

[27]  R. Austin,et al.  Collapse of DNA in ac electric fields. , 2011, Physical review letters.

[28]  S. Fischer,et al.  Salt-induced counterion-mobility anomaly in polyelectrolyte electrophoresis. , 2008, Physical review letters.

[29]  A. Ajdari,et al.  Electrohydrodynamic Patterns in Charged Colloidal Solutions , 1997 .

[30]  M. Washizu,et al.  Electrostatic manipulation of DNA in microfabricated structures , 1989, Conference Record of the IEEE Industry Applications Society Annual Meeting,.

[31]  J. Antosiewicz,et al.  Structure and dynamics of curved DNA fragments in solution: evidence for slow modes of configurational transitions. , 1993 .

[32]  M. Fixman Charged Macromolecules in External Fields. 2. Preliminary Remarks on the Cylinder , 1980 .

[33]  Rae M. Robertson,et al.  Diffusion of isolated DNA molecules: dependence on length and topology. , 2006, Proceedings of the National Academy of Sciences of the United States of America.

[34]  F. Oosawa Counterion fluctuation and dielectric dispersion in linear polyelectrolytes , 1970 .

[35]  Yingxi Zhu,et al.  Manipulating single annealed polyelectrolyte under alternating current electric fields: Collapse versus accumulation. , 2012, Biomicrofluidics.

[36]  J. Sturm,et al.  A nanofluidic railroad switch for DNA. , 2006, Nano letters.

[37]  J. Prost,et al.  Segregation in DNA solutions induced by electric fields , 1995, Science.

[38]  M. Mandel,et al.  Dielectric increment and dielectric dispersion of solutions containing simple charged linear macromolecules. I. Theory. , 1974, Biophysical chemistry.

[39]  J. McTague,et al.  Electric Polarization of Solutions of Rodlike Polyelectrolytes , 1966 .

[40]  E. Maginn,et al.  Molecular Simulation of Polyelectrolye Conformational Dynamics under an AC Electric Field , 2010 .

[41]  J. Thayer,et al.  Introduction to Analysis of Variance , 2001 .

[42]  DNA condensation by field-induced non-equilibrium noise. , 2009, Chemphyschem : a European journal of chemical physics and physical chemistry.

[43]  Nonlinear effects on electrokinetics of a highly charged porous sphere , 2014, Colloid and Polymer Science.

[44]  J. Hermans Sedimentation and electrophoresis of porous spheres , 1955 .

[45]  Cheng-Han Lee,et al.  Stretching DNA by electric field and flow field in microfluidic devices: An experimental validation to the devices designed with computer simulations. , 2013, Biomicrofluidics.

[46]  D. Porschke,et al.  The mechanism of ion polarisation along DNA double helices. , 1985, Biophysical chemistry.

[47]  A. Khokhlov,et al.  "Swiss-cheese" polyelectrolyte gels as media with extremely inhomogeneous distribution of charged species. , 2004, The Journal of chemical physics.

[48]  A. Ajdari,et al.  Electrohydrodynamic patterns in macroion dispersions under a strong electric field , 1997 .

[49]  S Tomić,et al.  Dielectric relaxation of DNA aqueous solutions. , 2007, Physical review. E, Statistical, nonlinear, and soft matter physics.

[50]  I. Noda,et al.  Transport phenomena of polyelectrolytes in solution under electric field , 1972 .

[51]  S. Diekmann,et al.  Thresholds in field-induced reactions of linear biopolymers. Strong chain-length dependence of field effects in DNA. , 1982, Biophysical chemistry.

[52]  S. A. Ruiz,et al.  Shape anisotropy of a single random-walk polymer. , 2000, Proceedings of the National Academy of Sciences of the United States of America.

[53]  B. Nordén,et al.  Orientation of large DNA during free solution electrophoresis studied by linear dichroism , 1993 .

[54]  J. Overbeek,et al.  Electrophoresis of polyelectrolytes with partial drainage , 1956 .

[55]  P. Gennes,et al.  Dynamics of confined polymer chains , 1977 .

[56]  R. M. Fuoss,et al.  Wien Effect in Polyelectrolytes , 1952 .

[57]  D. Porschke,et al.  Threshold effects observed in conformation changes induced by electric fields , 1976, Biopolymers.

[58]  T. Duke,et al.  Electrohydrodynamic Stretching of DNA in Confined Environments , 1998 .

[59]  C. Houssier,et al.  ELECTROOPTIC EFFECTS ON NUCLEIC ACIDS AND NUCLEOPROTEINS. , 1964, Biochimica et biophysica acta.

[60]  L. Onsager,et al.  Wien Effect in Simple Strong Electrolytes , 1957 .

[61]  Hsueh-Chia Chang,et al.  Hysteretic Conformational Transition of Single Flexible Polyelectrolyte under Resonant AC Electric Polarization , 2010 .

[62]  Ulrich W. Suter,et al.  Shape of unperturbed linear polymers: polypropylene , 1985 .

[63]  Patrick S. Doyle,et al.  Compression and self-entanglement of single DNA molecules under uniform electric field , 2011, Proceedings of the National Academy of Sciences.

[64]  Joshua H. Carpenter,et al.  Fluctuation modes of nanoconfined DNA. , 2012, Journal of applied physics.

[65]  Douglas R. Tree,et al.  Is DNA a Good Model Polymer? , 2013, Macromolecules.

[66]  D. Hoagland,et al.  Capillary Electrophoresis Measurements of the Free Solution Mobility for Several Model Polyelectrolyte Systems , 1999 .