Molecular Dynamics Study of the Effect of L-Alanine Chiral Dopants on Diluted Chromonic Solutions
OMM Rivas and AD Rey, JOURNAL OF PHYSICAL CHEMISTRY B, 123, 8995-9010 (2019).
DOI: 10.1021/acs.jpcb.9b06111
Atomistic molecular dynamics simulations have been performed for disodium cromoglycate (DSCG) chromonic solutions mixed with L-alanine chiral dopants. We study the fundamental molecular mechanisms induced by low concentrations of L-alanine on diluted DSCG solutions, including their effect on the chromonic aggregates, the solvent, and sodium counterions. Simulations reveal that Lalanine molecules primarily interact with DSCG stacks establishing salt bridges between their respective ammonium and carboxylate groups. Our results demonstrate that L-alanine and sodium counterions jointly establish an intricate network of noncovalent interactions around DSCG aggregates that decreases the global electrostatic repulsion of the chromonic system. Two possible structural effects in DSCG aggregates arise from this electronic stabilization: the increment of the total number of consecutively stacked aromatic planes per DSCG aggregate (intracolumnar effect) or the partial separation reduction between neighboring DSCG columnar sections due to the simultaneous bridging of intercolumnar DSCG carboxylate sites by sodium counterions, forming sodium bridges (intercolumnar effect). Sodium bridges may be responsible for the formation of stacking faults in DSCG aggregates in the form of lateral overlap junctions. This mechanism would explain the difference between lower X-ray correlation lengths with the expected persistence length in chromonics.
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