Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userA variational approach to necklaces formation in polyelectrolytes
149
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
By means of a variational approach we study the conditions under which a polyelectrolyte in a bad solvent will undergo a transition from a rod-like structure to a ``necklace structure in which the chain collapses into a series of globules joined by stretched chain segments.
rate research
Read More
We analyze, by means of an RPA calculation, the conditions under which a mixture of oppositely charged polyelectrolytes can micro-segregate in the neighborhood of a charged surface creating a layered structure. A number of stable layers can be formed if the surface is sufficiently strongly charged even at temperatures at which the bulk of the mixture is homogeneous.
The collapse of flexible polyelectrolytes in a solution of multivalent counterions is studied by means of a two state model. The states correspond to rod-like and spherically collapsed conformations respectively. We focus on the very dilute monomer concentration regime where the collapse transition is found to occur when the charge of the multivalent salt is comparable (but smaller) to that of the monomers. The main contribution to the free energy of the collapsed conformation is linear in the number of monomers $N$, since the internal state of the collapsed polymer approaches that of an amorphous ionic solid. The free energy of the rod-like state grows as $Nln N$, due to the electrostatic energy associated with that shape. We show that practically all multivalent counterions added to the system are condensed into the polymer chain, even before the collapse.
Polyelectrolytes such as single and double stranded DNA and many synthetic polymers undergo two structural transitions upon increasing the concentration of multivalent salt or molecules. First, the expanded-stretched chains in low monovalent salt solutions collapse into nearly neutral compact structures when the density of multivalent salt approaches that of the monomers. With further addition of multivalent salt the chains redissolve acquiring expanded-coiled conformations. We study the redissolution transition using a two state model [F. Solis and M. Olvera de la Cruz, {it J. Chem. Phys.} {bf 112} (2000) 2030]. The redissolution occurs when there is a high degree of screening of the electrostatic interactions between monomers, thus reducing the energy of the expanded state. The transition is determined by the chemical potential of the multivalent ions in the solution $mu$ and the inverse screening length $kappa$. The transition point also depends on the charge distribution along the chain but is almost independent of the molecular weight and degree of flexibility of the polyelectrolytes. We generate a diagram of $mu$ versus $kappa^2$ where we find two regions of expanded conformations, one with charged chains and other with overcharged (inverted charge) chains, separated by a collapsed nearly neutral conformation region. The collapse and redissolution transitions occur when the trajectory of the properties of the salt crosses the boundaries between these regions. We find that in most cases the redissolution occurs within the same expanded branch from which the chain precipitates.
Recent advances in qubit fidelity and hardware availability have driven efforts to simulate molecular systems of increasing complexity in a quantum computer and motivated us to to design quantum algorithms for solving the electronic structure of periodic crystalline solids. To this effect, we present a hybrid quantum-classical algorithm based on Variational Quantum Deflation [Higgott et al., Quantum, 2019, 3, 156] and Quantum Phase Estimation [Dobv{s}iv{c}ek et al., Phys. Rev. A, 2007, 76, 030306(R)] to solve the band structure of any periodic system described by an adequate tight-binding model. We showcase our algorithm by computing the band structure of a simple-cubic crystal with one $s$ and three $p$ orbitals per site (a simple model for Polonium) using simulators with increasingly realistic levels of noise and culminating with calculations on IBM quantum computers. Our results show that the algorithm is reliable in a low-noise device, functional with low precision on present-day noisy quantum computers, and displays a complexity that scales as $Omega(M^3)$ with the number $M$ of tight-binding orbitals per unit-cell, similarly to its classical counterparts. Our simulations offer a new insight into the quantum mindset applied to solid state systems and suggest avenues to explore the potential of quantum computing in materials science.
We study the attractive interactions between rod-like charged polymers in solution that appear in the presence of multi-valence counterions. The counterions condensed to the rods exhibit both a strong transversal polarization and a longitudinal crystalline arrangement. At short distances between the rods, the fraction of condensed counterions increases, and the majority of these occupy the region between the rods, where they minimize their repulsive interactions by arranging themselves into packing structures. The attractive interaction is strongest for multivalent counterions. Our model takes into account the hard-core volume of the condensed counterions and their angular distribution around the rods. The hard core constraint strongly suppresses longitudinal charge fluctuations.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
