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Spectroscopic ellipsometry as a route to thermodynamic characterization.

Ronald P White1, Dragos Buculei2, Alexia M J M Beale2

  • 1Department of Chemistry, Dartmouth College, Hanover, New Hampshire, 03755, USA. jane.e.g.lipson@dartmouth.edu.

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Spectroscopic ellipsometry accurately measures the thermal expansion coefficient (α) in polymers using minimal sample. This optical technique advances thermodynamic characterization and material property prediction.

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Area of Science:

  • Materials Science
  • Polymer Science
  • Thermodynamics

Background:

  • Synthesizing molecularly designed materials outpaces thermodynamic characterization methods.
  • Connecting molecular structure to material properties requires accurate thermodynamic data.
  • Traditional methods for obtaining thermodynamic quantities like thermal expansion coefficient (α) often demand large sample sizes or complex experimental setups.

Purpose of the Study:

  • To establish spectroscopic ellipsometry as a viable method for thermodynamic characterization of materials.
  • To clarify the relationship between ellipsometric and volumetric thermal expansion coefficients.
  • To demonstrate the utility of ellipsometry-derived data for theoretical modeling and material design.

Main Methods:

  • Utilized spectroscopic ellipsometry, an optical technique for thin film analysis, to measure thermodynamic data.
  • Analyzed temperature-dependent data for ten polymers using both ellipsometry and macro-scale dilatometry.
  • Investigated the influence of substrate mechanical confinement on thin film thermal expansion.

Main Results:

  • Achieved excellent correlation between thermal expansion coefficients (α) obtained via ellipsometry and dilatometry, accounting for substrate effects.
  • Demonstrated that ellipsometry-derived α can predict polymer free volume using locally correlated lattice theory.
  • Discovered a linear correlation between the thermal expansion coefficient at the glass transition temperature (Tg) and Tg itself.

Conclusions:

  • Spectroscopic ellipsometry offers a straightforward method for thermodynamic characterization using minimal sample quantities.
  • This technique significantly expands the range of systems amenable to thermodynamic analysis.
  • Ellipsometry advances the prediction of material miscibility and dynamic relaxation, underpinning materials synthesis and property design.