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The excess electron at polyethylene interfaces.

Fernan Saiz1, David Cubero, Nick Quirke

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|July 28, 2018
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Summary
This summary is machine-generated.

Excess electrons in polyethylene prefer small nanovoids under 1 nm, according to Lanczos diagonalization. Density functional theory (DFT) suggests larger nanovoids, over 1 nm, for electron localization at interfaces.

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Area of Science:

  • Materials Science
  • Computational Chemistry
  • Condensed Matter Physics

Background:

  • Excess electrons in polymers like polyethylene exhibit unique properties.
  • Understanding electron behavior at polymer-vacuum interfaces is crucial for material design.

Purpose of the Study:

  • To investigate the energy and spatial properties of excess electrons in bulk and interfacial polyethylene.
  • To compare different computational methods for simulating electron behavior.

Main Methods:

  • Pseudopotential single-electron method (Lanczos diagonalization).
  • Density functional theory (DFT) with pseudopotentials/plane waves and local-density approximation.
  • DFT with all-electron Gaussian basis functions at the B3LYP level, including ghost atoms.

Main Results:

  • All three methods indicated similar spatial localization patterns for excess electrons.
  • Lanczos diagonalization predicted localization in nanovoids < 1 nm.
  • DFT suggested localization on surfaces in nanovoids > 1 nm.

Conclusions:

  • Orbital-based methods offer a valuable representation of excess electron properties in DFT studies of polyethylene/vacuum interfaces.
  • Discrepancies between Lanczos and DFT highlight the need for careful method selection in simulations.