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Area of Science:

  • Soft Matter Physics
  • Polymer Science
  • Biophysics

Background:

  • Complex coacervates and complex coacervate core micelles (C3Ms) are formed by mixing polyanions like single-stranded DNA (ssDNA) with polycations or cationic-neutral diblock copolymers.
  • Dynamics are crucial in these systems, but the effect of chain length on dynamics remains incompletely understood.
  • ssDNA offers a tunable platform to study chain length effects due to its monodispersity and adaptable length.

Purpose of the Study:

  • To investigate the dynamics of fluorescently labeled ssDNA within complex coacervate droplets and C3Ms.
  • To elucidate the influence of ssDNA chain length on dynamics in these condensed phases.
  • To understand the molecular exchange mechanisms in C3Ms and identify factors affecting exchange rates.

Main Methods:

  • Fluorescence Recovery After Photobleaching (FRAP) to probe ssDNA dynamics in complex coacervate droplets.
  • Förster Resonance Energy Transfer (FRET) to measure molecular exchange in C3Ms.
  • Langevin dynamics simulations to complement experimental FRET measurements.

Main Results:

  • ssDNA diffusion in complex coacervates shows a stronger dependence on DNA length than predicted by the sticky Rouse model, partly due to density changes.
  • Molecular exchange rates in C3Ms exhibit a broad distribution, primarily caused by chain length polydispersity.
  • Dye interactions significantly affect C3M exchange rates, and a new model is needed to describe C3M exchange, considering core species length.

Conclusions:

  • Chain length is a critical factor influencing ssDNA dynamics in both complex coacervates and C3Ms.
  • Polydispersity and dye-ligand interactions are key determinants of molecular exchange rates in C3Ms.
  • Findings advance the understanding of dynamics in DNA-based coacervates and provide insights for designing future soft matter systems.