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Area of Science:

  • Materials Science
  • Supramolecular Chemistry
  • Nanotechnology

Background:

  • Achieving ordered out-of-equilibrium states from homogeneous mixtures is a key challenge.
  • External energy sources like chemical fuels or light are commonly used for such separations.
  • Heat offers a promising, alternative energy source for controlling self-assembly processes.

Purpose of the Study:

  • To develop a temperature-controlled method for cycling between ordered and disordered states in a mixture of self-assembling building blocks.
  • To investigate the mechanism of building block exchange in self-assembled nanocubes.
  • To explore the influence of encapsulated guest molecules on the scrambling dynamics.

Main Methods:

  • Utilizing a mixture of two distinct building blocks that self-assemble into cubic structures (nanocubes).
  • Implementing a temperature-controlled cycle (25°C to 100°C) to induce transitions between disordered and ordered states.
  • Analyzing the scrambling of building blocks via the exchange of dissociated free building blocks.

Main Results:

  • A thermodynamically stable disordered state (statistical mixture of nanocubes) exists at lower temperatures (25°C).
  • Homoleptic assemblies (single-component nanocubes) are preferentially formed at higher temperatures (100°C) upon rapid cooling.
  • The rate of building block scrambling can be precisely controlled—accelerated, retarded, or blocked—by guest molecules encapsulated within the nanocubes.

Conclusions:

  • A heat-driven cycle enables reversible control over the order and disorder of self-assembled nanocube mixtures.
  • The scrambling mechanism is mediated by the exchange of dissociated building blocks.
  • Encapsulated guest molecules provide a tunable handle to modulate the dynamics of self-assembly and disassembly.