Compression and self-entanglement of single DNA molecules under uniform electric field

We experimentally study the effects of a uniform electric field on the conformation of single DNA molecules. We demonstrate that a moderate electric field (∼200 V/cm) strongly compresses isolated DNA polymer coils into isotropic globules. Insight into the nature of these compressed states is gained by following the expansion of the molecules back to equilibrium after halting the electric field. We observe two distinct types of expansion modes: a continuous molecular expansion analogous to a compressed spring expanding, and a much slower expansion characterized by two long-lived metastable states. Fluorescence microscopy and stretching experiments reveal that the metastable states are the result of intramolecular self-entanglements induced by the electric field. These results have broad importance in DNA separations and single molecule genomics, polymer rheology, and DNA-based nanofabrication.

[1]  R. Netz Nonequilibrium unfolding of polyelectrolyte condensates in electric fields. , 2003, Physical review letters.

[2]  D. Macconnell Be Stars in Open Clusters. , 1967 .

[3]  Robert Riehn,et al.  Restriction mapping in nanofluidic devices. , 2005, Proceedings of the National Academy of Sciences of the United States of America.

[4]  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.

[5]  R. Xu,et al.  Transient electric birefringence of N4 DNA (71 kb) in solution , 1990 .

[6]  Cees Dekker,et al.  Direct force measurements on DNA in a solid-state nanopore , 2006 .

[7]  P. Doyle,et al.  Conformational Preconditioning by Electrophoresis of DNA through a Finite Obstacle Array , 2008 .

[8]  Yitzhak Rabin,et al.  Metastable tight knots in a wormlike polymer. , 2007, Physical review letters.

[9]  Christian H. Reccius,et al.  Compression and free expansion of single DNA molecules in nanochannels. , 2005, Physical review letters.

[10]  N. Sasaki,et al.  Slow Expansion of a Single Polymer Chain from the Knotted Globule , 2004 .

[11]  Stephen R Quake,et al.  Behavior of complex knots in single DNA molecules. , 2003, Physical review letters.

[12]  J. Viovy Electrophoresis of DNA and other polyelectrolytes: Physical mechanisms , 2000 .

[13]  K. Dorfman DNA electrophoresis in microfabricated devices , 2010 .

[14]  G. Fredrickson The theory of polymer dynamics , 1996 .

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

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

[17]  Victor Steinberg,et al.  Concentration dependence of the longest relaxation times of dilute and semi-dilute polymer solutions , 2009 .

[18]  F. Sor,et al.  Irreversible trapping of DNA during crossed‐field gel electrophoresis , 1992, Electrophoresis.

[19]  Daniel W. Trahan,et al.  Coil-stretch Transition of DNA Molecules in Slit-like Confinement. , 2010, Macromolecules.

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

[21]  D. Jary,et al.  Nonlinear viscoelasticity of entangled DNA molecules , 1999 .

[22]  Toyoichi Tanaka,et al.  Metastable globules in good solvents: Topologically stabilized state of polymers , 1995 .

[23]  P. Doyle,et al.  Studying confined polymers using single-molecule DNA experiments , 2008 .

[24]  C H Wiggins,et al.  Dynamic patterns and self-knotting of a driven hanging chain. , 2001, Physical review letters.

[25]  M. Bazant,et al.  Nonlinear electrokinetics at large voltages , 2009 .

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

[27]  Gaurav Arya,et al.  Biophysics of knotting. , 2010, Annual review of biophysics.

[28]  M. Vázquez,et al.  Knotting probability of DNA molecules confined in restricted volumes: DNA knotting in phage capsids , 2002, Proceedings of the National Academy of Sciences of the United States of America.

[29]  C. Abrams,et al.  Swelling dynamics of collapsed polymers , 2004 .

[30]  N. Yoshinaga Folding and unfolding kinetics of a single semiflexible polymer. , 2008, Physical review. E, Statistical, nonlinear, and soft matter physics.

[31]  C Micheletti,et al.  Biopolymer organization upon confinement , 2010, Journal of physics. Condensed matter : an Institute of Physics journal.

[32]  C. Abrams,et al.  Arrested swelling of highly entangled polymer globules. , 2003, Physical review letters.

[33]  Igor M. Sokolov,et al.  Diffusion mechanisms of localised knots along a polymer , 2006, cond-mat/0609514.

[34]  Harold G. Craighead,et al.  Revisiting the Conformation and Dynamics of DNA in Slitlike Confinement , 2010 .

[35]  Self-similar chain conformations in polymer gels , 1999, Physical review letters.

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

[37]  Dorian M. Raymer,et al.  Spontaneous knotting of an agitated string , 2007, Proceedings of the National Academy of Sciences.

[38]  P. Stączek,et al.  Gyrase and Topo IV modulate chromosome domain size in vivo , 1998, Molecular microbiology.

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