ࡱ> xzqrstuvw`  5bjbjss s@Q'$P.Dr$)@"E(G(G(G(G(G(G($N*h,pk(]k((###E(#E(##:m&,& >Nps! & 'L(0)&.&-"&-&&-&(m#[0k(k(#X)$    FUNDAMENTAL LENGTH SCALES IN SEMIDILUTE Na-DNA SOLUTIONS S.Tomi1,* , T.Vuleti1, S.Dolanski Babi1,2, T.Ivek1, S.Kr a3, L.Gripari4 and R.Podgornik5 1Institut za fiziku, Zagreb, Croatia 2 School of Medicine, University of Zagreb, Croatia 3 Institut Ruer Boakovi, Zagreb, Croatia 4Dept. of Biological Chemistry, UCLA School of Medicine, Los Angeles, USA 5Department of Physics, University of Ljubljana and J.Stefan Institute, Ljubljana, Slovenia and Laboratory of Physical and Structural Biology NICHD, National Institutes of Health, Bethesda, MD  HYPERLINK "mailto:*stomic@ifs.hr" *stomic@ifs.hr Charged polymers are ubiquitous in colloidal systems and soft matter in general [1] and play a fundamental role in determining the structure of various (macro)molecular assemblies. Deoxyribonucleic acid (DNA) is, in many respects, a paradigm of a stiff, highly charged polymer [2] where this complex behavior has been studied in great detail. Electrostatic interactions for a single stiff polyelectrolyte chain such as DNA with monovalent counterions and added salt in aqueous solutions are reasonably well understood and are standardly approached via the Poisson - Boltzmann theory that combines electrostatics with statistical mechanics of mobile ionic species on a simplified mean-field level. The coupling between structure and interactions in the semidilute polyelectrolyte solutions composed of many chains, their respective counterions and added salt is a more complicated matter and a theoretical consensus is much less well established than in the case of a single polyelectrolyte chain or semidilute solutions of neutral polymers [3]. There are several fundamental concepts and length scales in the theoretical understanding of either a single charged polymer chain or semidilute solutions of many charged polymer chains: the Manning-Oosawa counterion condensation, the Odijk-Skolnick-Fixman electrostatic persistence length and the de Gennes-Pfeuty-Dobrynin correlation length of a semidilute polyelectrolyte solution [3,4,5]. In order to study the fundamental length scales in semidilute solutions, we have undertaken an investigation of dielectric relaxation properties of Na-DNA aqueous solutions that covers a broad range of DNA concentrations, as well as added salt concentrations [6,7]. We have used low-frequency dielectric spectroscopy technique in the frequency range 40 Hz - 110 MHz, widely established as a direct and non-destructive tool to probe charged entities and their structure in various bio-macromolecular systems [8]. Our aim was not only to verify the predictions of the various theories in the well defined conditions, but also to investigate the behavior of DNA at extreme conditions like very low and very high added salt limit. Results revealed two broad relaxation modes of strength 20 < DeLF <100 and 5 < DeHF <20, centered at 0.5 kHz < nLF < 70 kHz and 0.1 MHz< nHF <15 MHz (Figure 1). The characteristic length scale of the LF process, 50 <LLF <750 nm, varies with the concentration of DNA as cDNA-0.25 and is independent of the ionic strength in the low added salt regime. Conversely, it does not vary with the concentration of DNA, but depends on the ionic strength of the added salt as Is-1 in the high added salt regime. These features suggest that the corresponding length scale can be identified as an average size of the Gaussian chain composed of correlation blobs in the low added salt limit, and as the Odijk-Skolnick-Fixman value of the single chain persistence length in the high added salt limit. On the other hand, the characteristic length scale of the HF process for intermediate and large DNA concentrations.can be identified as de Gennes - Pfeuty Dobrynin correlation length of polyelectrolytes in semidilute solution, which varies with the concentration of DNA as cDNA-0.5 and is independent of the ionic strength in the low added salt regime. At low DNA concentrations and in the low added salt limit the characteristic length scale of the HF process scales as cDNA-0.33. We put these results in perspective regarding the integrity of the double stranded form of DNA at low salt conditions as well as regarding the role of different types of counterions in different regimes of dielectric dispersion. We also suggest theoretical interpretations for all these length scales in the whole regime of DNA and salt concentrations and discuss their ramifications and limitations.  Figure 1 Double logarithmic plot of the frequency dependence of the imaginary part of the dielectric function (e  ) at T=25(C of (a) pure water DNA solutions (for DNA concentrations a1-a4: 2.5, 0.4, 0.1, 0.0125 mg/mL) and (b) DNA solutions with added salt Is= 1mM (for DNA concentrations b1-b4: 0.83, 0.5, 0.31, 0.125 mg/mL). The full lines are fits to the sum of twon |   ( , . 0 F x z ̾vk]vhwhw6CJ]aJhw6CJ]aJhwhwCJH*aJhK[UCJaJhp5CJH*aJhp5CJaJhh5CJaJhhf(5CJaJhf(CJaJhh5CJH*aJhf(h5>*CJaJh hK[UCJhK[UB*OJQJ^JaJphjhK[UUhK[Ul n   , . x 6 " >[gd%`gds`gdw$a$gdwgdf(gdgd$a$ $hL^h`La$45z | 6 8 8XYǻᔩ{sohdo`o`o`od`\X`oh5{ch~qahXhW hhhhK[U6\]hwhwaJhwhw0J6CJ]aJ)j(hwhw6CJU]aJ#jhwhw6CJU]aJhwhw6CJaJhwhw6CJH*aJhwhwCJH*aJhwhw6CJ]aJ hwhw56CJ\]aJ!"/v}~`YZ[bik$(,4<bdfjlnp,46:½ʹҨғғҏΏ҈҄hNV, hIh^mhwh# h#H*h#OJQJhhf h> H*h> OJQJh> h\tCH*h\tCOJQJh\tChDh^m hhh^mhxQ hIh%h%h8bKhWhh5{chp3:>@R\]I9:ixFe  NOPQRļĵħ񣧜{t hhjO)hhUhhCh* h}$H* h}$H* hIh}$h5{ch}$ hoG3H* hoG3H* hIhoG3hoG3hs hIhqhq h"pH* h"pH*h"phhH* hH* hIh^mh^m hNV,H* h^mH*+[MNOQR111111-22 3344444444  & F^gdOgd&gd!gd$a$gdygd^m`gdxQRZ[$& 0000000000000000000001㳧schowh BCJH*OJQJaJhowh BCJH*aJhowh BCJH*aJhowh BCJOJQJaJUhowh BCJaJhowh?MCJH*aJhowh?MCJaJ jhowhCJaJhowhCJOJQJaJhhF7CJaJhowhCJaJhowCJaJhow5CJaJ% Havriliak-Negami forms; the dashed lines represent the single Havriliak-Negami form e(w) - eHF = (e0 - eHF) / (1 + (iwt0)1-a). References F.Oosawa, Polyelectrolytes, Dekker, New York, 1971. V.A.Bloomfield, D.M.Crothers and I.Tinocco, Jr., Nucleic Acids, University Science Books, Sausalito, 2000. A.V.Dobrynin and M.Rubinstein, Prog.Polym.Sci. 2005, 30, 1049; A.V.Dobrynin, R.H.Colby and M.Rubinstein, Macromolecules 1995, 28, 1859. T.Odijk, J.Polym.Phys.B: Polym.Phys. 1977, 15, 477; J.Skolnick and M.Fixman, Macromolecules 1977, 10, 944. P.G.de Gennes, P.Pincus, R.M.Velasco and F.Brochard, J.Phys.(Paris), 1976, 37, 1461; P.Pfeuty, J.Phys.(Paris), 1978, 39, C2-149. S.Tomic, T.Vuletic, S.Dolanski Babic, S.Krca, D.Ivankovic, L.Griparic and R.Podgornik, Phys.Rev.Lett. 2006, 97, 098303. S.Tomic, S.Dolanski Babic, T.Vuletic, S.Krca, D.Ivankovic, L.Griparic and R.Podgornik, Phys.Rev.E 2007, 75, 021905. F.Bordi, C.Cametti and R.H.Colby, J.Phys.Condensed Matter 2004, 16, R1423.     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