Browsing by Author "Ala-Nissila, T."

Now showing 1 - 8 of 8

Open Access
Comment on 'Nonlocal statistical field theory of dipolar particles in electrolyte solutions'
(IOP, 2019) Büyükdağlı, Şahin; Ala-Nissila, T.; Blossey, R.
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.
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.
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.
Open Access
PH-mediated regulation of polymer transport through SiN pores
(Institute of Physics Publishing, 2018) Büyükdağlı, Şahin; Ala-Nissila, T.
We characterize the pH-controlled polymer capture and transport through silicon nitride (SiN) pores subject to protonation. A charge regulation model able to reproduce the experimental zeta potential of SiN pores is coupled with electrohydrodynamic polymer transport equations. The formalism can quantitatively explain the experimentally observed non-monotonic pH dependence of avidin conductivity in terms of the interplay between the electroosmotic and electrophoretic drag forces on the protein. We also scrutinize the DNA conductivity of SiN pores. We show that in the low-pH regime where the amphoteric pore is cationic, DNA-pore attraction acts as an electrostatic trap. This provides a favorable condition for fast polymer capture and extended translocation required for accurate polymer sequencing.
Open Access
Pulling a DNA molecule through a nanopore embedded in an anionic membrane: tension propagation coupled to electrostatics
(Institute of Physics Publishing, 2020) Sarabadani, J.; Büyükdağlı, Şahin; Ala-Nissila, T.
We consider the influence of electrostatic forces on driven translocation dynamics of a flexible polyelectrolyte being pulled through a nanopore by an external force on the head monomer. To this end, we augment the iso-flux tension propagation theory with electrostatics for a negatively charged biopolymer pulled through a nanopore embedded in a similarly charged anionic membrane. We show that in the realistic case of a single-stranded DNA molecule, dilute salt conditions characterized by weak charge screening, and a negatively charged membrane, the translocation dynamics is unexpectedly accelerated despite the presence of large repulsive electrostatic interactions between the polymer coil on the cis side and the charged membrane. This is due to the rapid release of the electrostatic potential energy of the coil during translocation, leading to an effectively attractive force that assists end-driven translocation. The speedup results in non-monotonic polymer length and membrane charge dependence of the exponent α characterizing the translocation time τ ∝ Nα 0 of the polymer with length N0. In the regime of long polymers N0 500, the translocation exponent exceeds its upper limit α = 2 previously observed for the same system without electrostatic interactions.
Open Access
Theoretical and computational analysis of the electrophoretic polymer mobility inversion induced by charge correlations
(American Physical Society, 2023-03-23) Yang, X.; Büyükdağlı, Şahin; Scacchi, A.; Sammalkorpi, M.; Ala-Nissila, T.
Electrophoretic (EP) mobility reversal is commonly observed for strongly charged macromolecules in multivalent salt solutions. This curious effect takes place, e.g., when a charged polymer, such as DNA, adsorbs excess counterions so that the counterion-dressed surface charge reverses its sign, leading to the inversion of the polymer drift driven by an external electric field. In order to characterize this seemingly counterintuitive phenomenon that cannot be captured by electrostatic mean-field theories, we adapt here a previously developed strong-coupling-dressed Poisson-Boltzmann approach to the cylindrical geometry of the polyelectrolyte-salt system. Within the framework of this formalism, we derive an analytical polymer mobility formula dressed by charge correlations. In qualitative agreement with polymer transport experiments, this mobility formula predicts that the increment of the monovalent salt, the decrease of the multivalent counterion valency, and the increase of the dielectric permittivity of the background solvent suppress charge correlations and increase the multivalent bulk counterion concentration required for EP mobility reversal. These results are corroborated by coarse-grained molecular dynamics simulations showing how multivalent counterions induce mobility inversion at dilute concentrations and suppress the inversion effect at large concentrations. This re-entrant behavior, previously observed in the aggregation of like-charged polymer solutions, calls for verification by polymer transport experiments.
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.