Browsing by Subject "Polymer translocation"
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Item Open Access Dielectric trapping of biopolymers translocating through insulating membranes(MDPI AG, 2018) Büyükdağlı, Şahin; Sarabadani, J.; Ala-Nissila, T.Sensitive sequencing of biopolymers by nanopore-based translocation techniques requires an extension of the time spent by the molecule in the pore. We develop an electrostatic theory of polymer translocation to show that the translocation time can be extended via the dielectric trapping of the polymer. In dilute salt conditions, the dielectric contrast between the low permittivity membrane and large permittivity solvent gives rise to attractive interactions between the cis and trans portions of the polymer. This self-attraction acts as a dielectric trap that can enhance the translocation time by orders of magnitude. We also find that electrostatic interactions result in the piecewise scaling of the translocation time t with the polymer length L. In the short polymer regime L ≲ 10 nm where the external drift force dominates electrostatic polymer interactions, the translocation is characterized by the drift behavior τ ~ L2. In the intermediate length regime 10 nm. ≲ L ≲ kb -1 where kb is the Debye-Hückel screening parameter, the dielectric trap takes over the drift force. As a result, increasing polymer length leads to quasi-exponential growth of the translocation time. Finally, in the regime of long polymers L ≳ kb -1 where salt screening leads to the saturation of the dielectric trap, the translocation time grows linearly as τ ~ L. This strong departure from the drift behavior highlights the essential role played by electrostatic interactions in polymer translocation.Item Open Access Electrostatics of Polymer Translocation Events in Electrolyte Solutions(American Institute of Physics Inc., 2016) Buyukdagli, S.; Ala-Nissila, T.We develop an analytical theory that accounts for the image and surface charge interactions between a charged dielectric membrane and a DNA molecule translocating through the membrane. Translocation events through neutral carbon-based membranes are driven by a competition between the repulsive DNA-image-charge interactions and the attractive coupling between the DNA segments on the trans and the cis sides of the membrane. The latter effect is induced by the reduction of the coupling by the dielectric membrane. In strong salt solutions where the repulsive image-charge effects dominate the attractive trans-cis coupling, the DNA molecule encounters a translocation barrier of ∼10 kBT. In dilute electrolytes, the trans-cis coupling takes over image-charge forces and the membrane becomes a metastable attraction point that can trap translocating polymers over long time intervals. This mechanism can be used in translocation experiments in order to control DNA motion by tuning the salt concentration of the solution.Item Open Access Electrostatics of polymer translocation through membrane nanopores in electrolyte solutions(2021-02) Mohamed, Ghada Mahmoud AbdullahThe transport of polymers across membranes in electrolyte solutions happens in most biological systems and is necessary for cells to function. Moreover, the poly-mer translocation process has proven to be very important in experiments and applications as well, providing a rich source of information about the polymer’s size and composition [1], [2], making the polymer translocation procedure a po-tential sequencing method that is efficient, cheap, and quick [3], [4]. However, no consensus on the theoretical understanding of the translocation mechanism has been reached yet [3], leaving it a major challenge for theoretical modelling due to its steric, hydrodynamic, and electrostatic interactions [2], [5]. Here, we calculate the electrostatic energy cost of the translocating polymer in both the approach and translocation phases and investigate the dependence of the poly-mer’s grand potential on different model tunable parameters. In the case of neu-tral membranes, low permittivity carbon-based membranes repel the approaching polymer with energy magnitude between ∼ 11 kBT and ∼ 27 kBT , while high permittivity engineered membranes attract the approaching polymer with almost the same energy magnitude. This behavior can be attributed to polymer image-charge interactions, which become amplified with low permittivity membranes. In strong salt solutions, the membrane exhibits a repulsive barrier that turns to a metastable well in dilute solutions. In pure solvents, the metastable well becomes a deep, stable well that traps the polymer in the pore for some time, where the translocation phase is mainly governed by the attractive trans-cis side interac-tion. For weakly charged membranes, the membrane charge attraction wins over the image-charge repulsion, leading to an attractive minimum at zt ≈ −1 nm followed by a repulsive barrier at lt = L/2 while for stronger membrane charges, the attractive well turns to a metastable point followed by an attractive, stable well. These results suggest that, in translocation experiments, DNA motion can be controlled by tuning the system parameters, such as the solution concentration or the membrane charge.Item Open Access Ionic current inversion in pressure-driven polymer translocation through nanopores(American Physical Society, 2015) Buyukdagli, S.; Blossey, R.; Ala-Nissila, T.We predict streaming current inversion with multivalent counterions in hydrodynamically driven polymer translocation events from a correlation-corrected charge transport theory including charge fluctuations around mean-field electrostatics. In the presence of multivalent counterions, electrostatic many-body effects result in the reversal of the DNA charge. The attraction of anions to the charge-inverted DNA molecule reverses the sign of the ionic current through the pore. Our theory allows for a comprehensive understanding of the complex features of the resulting streaming currents. The underlying mechanism is an efficient way to detect DNA charge reversal in pressure-driven translocation experiments with multivalent cations. © 2015 American Physical Society.Item Open Access Sensing translocating polymers via induced magnetic fields(TÜBİTAK, 2023) Büyükdağlı, ŞahinThe requirement to boost the resolution of nanopore-based biosequencing devices necessitates the integration of novel biosensing techniques with reduced sensitivity to background noise. In this article, we probe the signatures of translocating polymers in magnetic fields induced by ionic currents through membrane nanopores. Within the framework of a previously introduced charge transport theory, we evaluate the magnetic field signals generated by voltage- and pressure-driven DNA translocation events in monovalent salt solutions. Our formalism reveals that in voltage-driven transport, the translocating polymer suppresses the induced magnetic field via the steric blockage of the ion current through the midpore. In the case of pressure-driven transport, the magnetic field reduction by translocation originates from the negative electrokinetic contribution of the anionic DNA surface charges to the streaming current predominantly composed of salt cations. The magnitude of the corresponding field signals is located in the nano-Tesla range covered by the resolution of the magnetoelectric sensors able to detect magnetic fields down to the pico-Tesla range. This suggests that the integration of magnetic field detection techniques into the current biosequencing approaches can complement efficiently the conventional biosensing strategies employing ionic current readouts with high susceptibility to background noise.Item Open Access Theoretical modeling of polymer translocation: from the electrohydrodynamics of short polymers to the fluctuating long polymers(MDPI AG, 2019) Büyükdağlı, Şahin; Sarabadani, J.; Ala-Nissila, T.The theoretical formulation of driven polymer translocation through nanopores is complicated by the combination of the pore electrohydrodynamics and the nonequilibrium polymer dynamics originating from the conformational polymer fluctuations. In this review, we discuss the modeling of polymer translocation in the distinct regimes of short and long polymers where these two effects decouple. For the case of short polymers where polymer fluctuations are negligible, we present a stiff polymer model including the details of the electrohydrodynamic forces on the translocating molecule. We first show that the electrohydrodynamic theory can accurately characterize the hydrostatic pressure dependence of the polymer translocation velocity and time in pressure-voltage-driven polymer trapping experiments. Then, we discuss the electrostatic correlation mechanisms responsible for the experimentally observed DNA mobility inversion by added multivalent cations in solid-state pores, and the rapid growth of polymer capture rates by added monovalent salt in α-Hemolysin pores. In the opposite regime of long polymers where polymer fluctuations prevail, we review the iso-flux tension propagation (IFTP) theory, which can characterize the translocation dynamics at the level of single segments. The IFTP theory is valid for a variety of polymer translocation and pulling scenarios. We discuss the predictions of the theory for fully flexible and rodlike pore-driven and end-pulled translocation scenarios, where exact analytic results can be derived for the scaling of the translocation time with chain length and driving force.